Computational Modelling — Emerging class of SrZrS3 chalcogenide perovskite solar cells: Conductive MOFs as HTLs

237 measurement groups · 1,163 results

Reported values remain attached to the sample, method, conditions, extraction quality and source location that produced them.

SCAPS-1D parameter sweep

SCAPS SrZrS3 absorber layer model · Model

SrZrS3 carrier concentration, defect density and thickness were swept to optimize device performance.

Temperature: 300
Context: model
Measurement source: 5 · 3.2.1. Optimization of absorber carrier concentration, defect density, and thickness · Fig. 2

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
diffusion length range during absorber defect sweep	1.70E+00 to 1.70E-03	—	—	Text Range	5 · 3.2.1 · Fig. 2(g)
minority carrier lifetime range during absorber defect sweep	1.00E+05 to 1.00E-01	—	—	Text Range	5 · 3.2.1 · Fig. 2(g)
optimal absorber carrier concentrationMarked as a best value within this paper	10^17	—	—	Text Rounded Reported	5 · 3.2.1 · Fig. 2
optimal absorber defect densityMarked as a best value within this paper	10^12	—	—	Text Rounded Reported	5 · 3.2.1 · Fig. 2
optimal absorber thicknessMarked as a best value within this paper	600	—	—	Text Exact Reported	6 · 3.2.1 · Fig. 2
QE integral area range in absorber thickness sweep	52.41 to 83.4	—	—	Text Range	5 · 3.2.1 · Fig. 2(l)
Jsc range in absorber thickness sweep	16.24 to 27.67	—	—	Text Range	5 · 3.2.1 · Fig. 2(i-j)
PCE range in absorber thickness sweep	12.41 to 21.75	—	—	Text Range	5 · 3.2.1 · Fig. 2(i-j)

SCAPS-1D back metal work-function sweep

Cu-MOF:75 · Model

Back metal work function varied from 4.6 to 5.7 eV across optimized devices.

Temperature: 300
Context: model
Measurement source: 12 · 3.7. Impact of metal contacts · Figs. 10-12

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
Cu3(HHTP)2:24 maximum PCE after 5 eV BMWF	28.62	—	—	Text Exact Reported	12 · 3.7. Impact of metal contacts · Fig. 10
Cu-MOF PCE plateau threshold BMWF	5.2 eV	—	—	Text Exact Reported	12 · 3.7. Impact of metal contacts · Fig. 10
Fe2(DSBDC):21 peak PCE under BMWF sweep	29.28 % at 5.1 eV	—	—	Text Exact Reported	12 · 3.7. Impact of metal contacts · Fig. 10
Mn2(DSBDC):22 maximum PCE after 5 eV BMWF	29.22	—	—	Text Exact Reported	12 · 3.7. Impact of metal contacts · Fig. 10
NTU-9 PCE plateau threshold BMWF	5.5 eV	—	—	Text Exact Reported	12 · 3.7. Impact of metal contacts · Fig. 10
Sr-MOF:22 maximum PCE after 5 eV BMWF	28.43	—	—	Text Exact Reported	12 · 3.7. Impact of metal contacts · Fig. 10

SCAPS-1D energy-band alignment calculation

Cu3(HHTP)2:1 · Model

Initial device band offsets and activation energy at ETL/absorber and absorber/HTL interfaces.

Temperature: 300
Context: model
Measurement source: 13 · 3.6. Energy band diagram · Table 4

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
CBO at ETL/absorber interface	-0.3	—	—	Table Exact Reported	13 · 3.6. Energy band diagram · Table 4
activation energy at absorber/HTL interface	2.85	—	—	Table Exact Reported	13 · 3.6. Energy band diagram · Table 4
VBO at absorber/HTL interface	-0.15	—	—	Table Exact Reported	13 · 3.6. Energy band diagram · Table 4

SCAPS-1D energy-band alignment calculation

Cu3(HHTP)2:24 · Model

Optimized device band offsets and activation energy at ETL/absorber and absorber/HTL interfaces.

Temperature: 300
Context: model
Measurement source: 13 · 3.6. Energy band diagram · Table 4

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
CBO at ETL/absorber interface	-0.18	—	—	Table Exact Reported	13 · 3.6. Energy band diagram · Table 4
activation energy at absorber/HTL interface	2.85	—	—	Table Exact Reported	13 · 3.6. Energy band diagram · Table 4
VBO at absorber/HTL interface	-0.27	—	—	Table Exact Reported	13 · 3.6. Energy band diagram · Table 4

SCAPS-1D energy-band alignment calculation

Cu-MOF:1 · Model

Initial device band offsets and activation energy at ETL/absorber and absorber/HTL interfaces.

Temperature: 300
Context: model
Measurement source: 13 · 3.6. Energy band diagram · Table 4

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
CBO at ETL/absorber interface	-0.2	—	—	Table Exact Reported	13 · 3.6. Energy band diagram · Table 4
activation energy at absorber/HTL interface	1.22	—	—	Table Exact Reported	13 · 3.6. Energy band diagram · Table 4
VBO at absorber/HTL interface	-0.28	—	—	Table Exact Reported	13 · 3.6. Energy band diagram · Table 4

SCAPS-1D energy-band alignment calculation

Cu-MOF:75 · Model

Optimized device band offsets and activation energy at ETL/absorber and absorber/HTL interfaces.

Temperature: 300
Context: model
Measurement source: 13 · 3.6. Energy band diagram · Table 4

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
CBO at ETL/absorber interface	-0.2	—	—	Table Exact Reported	13 · 3.6. Energy band diagram · Table 4
activation energy at absorber/HTL interface	1.35	—	—	Table Exact Reported	13 · 3.6. Energy band diagram · Table 4
VBO at absorber/HTL interface	-0.42	—	—	Table Exact Reported	13 · 3.6. Energy band diagram · Table 4

SCAPS-1D energy-band alignment calculation

Fe2(DSBDC):1 · Model

Initial device band offsets and activation energy at ETL/absorber and absorber/HTL interfaces.

Temperature: 300
Context: model
Measurement source: 13 · 3.6. Energy band diagram · Table 4

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
CBO at ETL/absorber interface	-0.2	—	—	Table Exact Reported	13 · 3.6. Energy band diagram · Table 4
activation energy at absorber/HTL interface	1.92	—	—	Table Exact Reported	13 · 3.6. Energy band diagram · Table 4
VBO at absorber/HTL interface	-0.48	—	—	Table Exact Reported	13 · 3.6. Energy band diagram · Table 4

SCAPS-1D energy-band alignment calculation

Fe2(DSBDC):21 · Model

Optimized device band offsets and activation energy at ETL/absorber and absorber/HTL interfaces.

Temperature: 300
Context: model
Measurement source: 13 · 3.6. Energy band diagram · Table 4

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
CBO at ETL/absorber interface	0.01	—	—	Table Exact Reported	13 · 3.6. Energy band diagram · Table 4
activation energy at absorber/HTL interface	1.92	—	—	Table Exact Reported	13 · 3.6. Energy band diagram · Table 4
VBO at absorber/HTL interface	-0.3	—	—	Table Exact Reported	13 · 3.6. Energy band diagram · Table 4

SCAPS-1D energy-band alignment calculation

Mn2(DSBDC):1 · Model

Initial device band offsets and activation energy at ETL/absorber and absorber/HTL interfaces.

Temperature: 300
Context: model
Measurement source: 13 · 3.6. Energy band diagram · Table 4

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
CBO at ETL/absorber interface	-0.2	—	—	Table Exact Reported	13 · 3.6. Energy band diagram · Table 4
activation energy at absorber/HTL interface	2.6	—	—	Table Exact Reported	13 · 3.6. Energy band diagram · Table 4
VBO at absorber/HTL interface	-0.3	—	—	Table Exact Reported	13 · 3.6. Energy band diagram · Table 4

SCAPS-1D energy-band alignment calculation

Mn2(DSBDC):22 · Model

Optimized device band offsets and activation energy at ETL/absorber and absorber/HTL interfaces.

Temperature: 300
Context: model
Measurement source: 13 · 3.6. Energy band diagram · Table 4

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
CBO at ETL/absorber interface	-0.2	—	—	Table Exact Reported	13 · 3.6. Energy band diagram · Table 4
activation energy at absorber/HTL interface	2.6	—	—	Table Exact Reported	13 · 3.6. Energy band diagram · Table 4
VBO at absorber/HTL interface	-0.32	—	—	Table Exact Reported	13 · 3.6. Energy band diagram · Table 4

SCAPS-1D energy-band alignment calculation

NTU-9:1 · Model

Initial device band offsets and activation energy at ETL/absorber and absorber/HTL interfaces.

Temperature: 300
Context: model
Measurement source: 13 · 3.6. Energy band diagram · Table 4

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
CBO at ETL/absorber interface	-0.4	—	—	Table Exact Reported	13 · 3.6. Energy band diagram · Table 4
activation energy at absorber/HTL interface	1.72	—	—	Table Exact Reported	13 · 3.6. Energy band diagram · Table 4
VBO at absorber/HTL interface	-0.28	—	—	Table Exact Reported	13 · 3.6. Energy band diagram · Table 4

SCAPS-1D energy-band alignment calculation

NTU-9:22 · Model

Optimized device band offsets and activation energy at ETL/absorber and absorber/HTL interfaces.

Temperature: 300
Context: model
Measurement source: 13 · 3.6. Energy band diagram · Table 4

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
CBO at ETL/absorber interface	-0.4	—	—	Table Exact Reported	13 · 3.6. Energy band diagram · Table 4
activation energy at absorber/HTL interface	1.92	—	—	Table Exact Reported	13 · 3.6. Energy band diagram · Table 4
VBO at absorber/HTL interface	-0.3	—	—	Table Exact Reported	13 · 3.6. Energy band diagram · Table 4

SCAPS-1D energy-band alignment calculation

Sr-MOF:1 · Model

Initial device band offsets and activation energy at ETL/absorber and absorber/HTL interfaces.

Temperature: 300
Context: model
Measurement source: 13 · 3.6. Energy band diagram · Table 4

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
CBO at ETL/absorber interface	-0.2	—	—	Table Exact Reported	13 · 3.6. Energy band diagram · Table 4
activation energy at absorber/HTL interface	2.3	—	—	Table Exact Reported	13 · 3.6. Energy band diagram · Table 4
VBO at absorber/HTL interface	-0.3	—	—	Table Exact Reported	13 · 3.6. Energy band diagram · Table 4

SCAPS-1D energy-band alignment calculation

Sr-MOF:22 · Model

Optimized device band offsets and activation energy at ETL/absorber and absorber/HTL interfaces.

Temperature: 300
Context: model
Measurement source: 13 · 3.6. Energy band diagram · Table 4

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
CBO at ETL/absorber interface	-0.2	—	—	Table Exact Reported	13 · 3.6. Energy band diagram · Table 4
activation energy at absorber/HTL interface	2.3	—	—	Table Exact Reported	13 · 3.6. Energy band diagram · Table 4
VBO at absorber/HTL interface	-0.22	—	—	Table Exact Reported	13 · 3.6. Energy band diagram · Table 4

SCAPS-1D band-offset calculation

Cu-MOF:75 · Model

Cu-MOF electron affinity varied from 3.7 to 3.85 eV; CBO/VBO calculated at SrZrS3/Cu-MOF interface.

Temperature: 300
Context: model
Measurement source: 7 · 3.2.2.1. Influence of HTL's defect density and electron affinity · Table 3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
CBO at SrZrS3/Cu-MOF interface	0.35	—	—	Table Exact Reported	7 · 3.2.2.1. Influence of HTL's defect density and electron affinity · Table 3
VBO at SrZrS3/Cu-MOF interface	-0.53	—	—	Table Exact Reported	7 · 3.2.2.1. Influence of HTL's defect density and electron affinity · Table 3
CBO at SrZrS3/Cu-MOF interface	0.4	—	—	Table Exact Reported	7 · 3.2.2.1. Influence of HTL's defect density and electron affinity · Table 3
VBO at SrZrS3/Cu-MOF interface	-0.58	—	—	Table Exact Reported	7 · 3.2.2.1. Influence of HTL's defect density and electron affinity · Table 3
CBO at SrZrS3/Cu-MOF interface	0.25	—	—	Table Exact Reported	7 · 3.2.2.1. Influence of HTL's defect density and electron affinity · Table 3
VBO at SrZrS3/Cu-MOF interfaceMarked as a best value within this paper	-0.43	—	—	Table Exact Reported	7 · 3.2.2.1. Influence of HTL's defect density and electron affinity · Table 3
CBO at SrZrS3/Cu-MOF interface	0.3	—	—	Table Exact Reported	7 · 3.2.2.1. Influence of HTL's defect density and electron affinity · Table 3
VBO at SrZrS3/Cu-MOF interface	-0.48	—	—	Table Exact Reported	7 · 3.2.2.1. Influence of HTL's defect density and electron affinity · Table 3

SCAPS-1D HTL parameter sweep

SCAPS Cu-MOF HTL material model · Model

Cu-MOF HTL defect density, electron affinity, carrier concentration and thickness sweeps.

Temperature: 300
Context: model
Measurement source: 6-7 · 3.2.2. Optimization of HTL · Figs. 3-4

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
optimal Cu-MOF HTL carrier concentrationMarked as a best value within this paper	10^20	—	—	Text Rounded Reported	7 · 3.2.2.2 · Fig. 4
optimal Cu-MOF HTL defect densityMarked as a best value within this paper	10^12	—	—	Text Rounded Reported	6 · 3.2.2.1 · Fig. 3
optimal Cu-MOF electron affinityMarked as a best value within this paper	3.85	—	—	Text Exact Reported	7 · 3.2.2.1 · Fig. 3
optimal Cu-MOF HTL thicknessMarked as a best value within this paper	200	—	—	Text Exact Reported	7 · 3.2.2.2 · Fig. 4
Cu-MOF NIR QE improvement with HTL thickness	14 to 45	—	—	Text Range	7 · 3.2.2.2 · Fig. 4(g)

SCAPS-1D interface-defect density sweep

Cu-MOF:75 · Model

Neutral defects at SnO2/SrZrS3 and SrZrS3/Cu-MOF interfaces varied from 10^10 to 10^20 cm^-3.

Temperature: 300
Context: model
Measurement source: 13 · 3.8. Influence of interface properties · Fig. 13

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
recommended SrZrS3/Cu-MOF interface defect density rangeMarked as a best value within this paper	10^10 to 10^12	—	—	Text Range	13 · 3.8. Influence of interface properties · Fig. 13(c-d)
Jsc decline under SrZrS3/Cu-MOF defect sweep	26.34 to 22.44	—	—	Text Range	13 · 3.8. Influence of interface properties · Fig. 13(c-d)
PCE decline under SrZrS3/Cu-MOF defect sweep	30.60 to 15.76	—	—	Text Range	13 · 3.8. Influence of interface properties · Fig. 13(c-d)
Voc decline under SrZrS3/Cu-MOF defect sweep	1.17 to 0.78	—	—	Text Range	13 · 3.8. Influence of interface properties · Fig. 13(c-d)
optimal SnO2/SrZrS3 interface defect densityMarked as a best value within this paper	10^14	—	—	Text Rounded Reported	13 · 3.8. Influence of interface properties · Fig. 13(a-b)
PCE decline under SnO2/SrZrS3 defect sweep	30.60 to 24.52	—	—	Text Range	13 · 3.8. Influence of interface properties · Fig. 13(a-b)

SCAPS-1D J-V simulation

Cu3(HHTP)2:1 · Model

Initial c-MOF HTL device parameters before optimisation.

Temperature: 300
Geometry: FTO/SnO2/SrZrS3/c-MOF/back contact
Context: model
Measurement source: 9 · 3.3. Influence of different c-MOFs as HTL · Fig. 5(c-h)

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	57.29	—	—	Visual Estimate Approximate	9 · 3.3. Influence of different c-MOFs as HTL · Fig. 5(c-h)
short-circuit current density	22.11	—	—	Visual Estimate Approximate	9 · 3.3. Influence of different c-MOFs as HTL · Fig. 5(c-h)
power conversion efficiency	12.06	—	—	Text Exact Reported	9 · 3.3. Influence of different c-MOFs as HTL · Fig. 5(c-h)
open-circuit voltage	0.9523	—	—	Visual Estimate Approximate	9 · 3.3. Influence of different c-MOFs as HTL · Fig. 5(c-h)

SCAPS-1D J-V simulation

Cu3(HHTP)2:24 · Model

Best optimized c-MOF HTL device selected from 193 simulated configurations.

Temperature: 300
Geometry: FTO/SnO2/SrZrS3/Cu3(HHTP)2/Fe
Context: model
Measurement source: 17 · Table 5 · Table 5

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.48	—	—	Table Exact Reported	17 · Table 5 · Table 5
short-circuit current density	25.51	—	—	Table Exact Reported	17 · Table 5 · Table 5
power conversion efficiency	28.62	—	—	Table Exact Reported	17 · Table 5 · Table 5
open-circuit voltage	1.2677	—	—	SI Table Exact Reported	6 · Supplementary information · Table S3

SCAPS-1D J-V simulation

Cu-MOF:1 · Model

Initial c-MOF HTL device parameters before optimisation.

Temperature: 300
Geometry: FTO/SnO2/SrZrS3/c-MOF/back contact
Context: model
Measurement source: 9 · 3.3. Influence of different c-MOFs as HTL · Fig. 5(c-h)

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	54.88	—	—	Visual Estimate Approximate	9 · 3.3. Influence of different c-MOFs as HTL · Fig. 5(c-h)
short-circuit current density	23.36	—	—	Visual Estimate Approximate	9 · 3.3. Influence of different c-MOFs as HTL · Fig. 5(c-h)
power conversion efficiency	11.03	—	—	Text Exact Reported	9 · 3.3. Influence of different c-MOFs as HTL · Fig. 5(c-h)
open-circuit voltage	0.8603	—	—	Visual Estimate Approximate	9 · 3.3. Influence of different c-MOFs as HTL · Fig. 5(c-h)

SCAPS-1D J-V simulation

Cu-MOF:75 · Model

Best optimized c-MOF HTL device selected from 193 simulated configurations.

Temperature: 300
Geometry: FTO/SnO2/SrZrS3/Cu-MOF/Ni
Context: model
Measurement source: 17 · Table 5 · Table 5

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.4	—	—	Table Exact Reported	17 · Table 5 · Table 5
short-circuit current density	29.54	—	—	Table Exact Reported	17 · Table 5 · Table 5
power conversion efficiencyMarked as a best value within this paper	30.6	—	—	Table Exact Reported	17 · Table 5 · Table 5
open-circuit voltage	1.1720	—	—	SI Table Exact Reported	6 · Supplementary information · Table S3

SCAPS-1D J-V simulation

Fe2(DSBDC):1 · Model

Initial c-MOF HTL device parameters before optimisation.

Temperature: 300
Geometry: FTO/SnO2/SrZrS3/c-MOF/back contact
Context: model
Measurement source: 9 · 3.3. Influence of different c-MOFs as HTL · Fig. 5(c-h)

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	58.14	—	—	Visual Estimate Approximate	9 · 3.3. Influence of different c-MOFs as HTL · Fig. 5(c-h)
short-circuit current density	24.26	—	—	Visual Estimate Approximate	9 · 3.3. Influence of different c-MOFs as HTL · Fig. 5(c-h)
power conversion efficiency	12.66	—	—	Text Exact Reported	9 · 3.3. Influence of different c-MOFs as HTL · Fig. 5(c-h)
open-circuit voltage	0.8973	—	—	Visual Estimate Approximate	9 · 3.3. Influence of different c-MOFs as HTL · Fig. 5(c-h)

SCAPS-1D J-V simulation

Fe2(DSBDC):21 · Model

Best optimized c-MOF HTL device selected from 193 simulated configurations.

Temperature: 300
Geometry: FTO/SnO2/SrZrS3/Fe2(DSBDC)/Fe
Context: model
Measurement source: 17 · Table 5 · Table 5

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.5	—	—	Table Exact Reported	17 · Table 5 · Table 5
short-circuit current density	25.59	—	—	Table Exact Reported	17 · Table 5 · Table 5
power conversion efficiency	28.29	—	—	Table Exact Reported	17 · Table 5 · Table 5
open-circuit voltage	1.2491	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D J-V simulation

Mn2(DSBDC):1 · Model

Initial c-MOF HTL device parameters before optimisation.

Temperature: 300
Geometry: FTO/SnO2/SrZrS3/c-MOF/back contact
Context: model
Measurement source: 9 · 3.3. Influence of different c-MOFs as HTL · Fig. 5(c-h)

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	58.58	—	—	Visual Estimate Approximate	9 · 3.3. Influence of different c-MOFs as HTL · Fig. 5(c-h)
short-circuit current density	24.16	—	—	Visual Estimate Approximate	9 · 3.3. Influence of different c-MOFs as HTL · Fig. 5(c-h)
power conversion efficiency	13.25	—	—	Text Exact Reported	9 · 3.3. Influence of different c-MOFs as HTL · Fig. 5(c-h)
open-circuit voltage	0.9361	—	—	Visual Estimate Approximate	9 · 3.3. Influence of different c-MOFs as HTL · Fig. 5(c-h)

SCAPS-1D J-V simulation

Mn2(DSBDC):22 · Model

Best optimized c-MOF HTL device selected from 193 simulated configurations.

Temperature: 300
Geometry: FTO/SnO2/SrZrS3/Mn2(DSBDC)/Fe
Context: model
Measurement source: 17 · Table 5 · Table 5

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.45	—	—	Table Exact Reported	17 · Table 5 · Table 5
short-circuit current density	25.52	—	—	Table Exact Reported	17 · Table 5 · Table 5
power conversion efficiency	28.8	—	—	Table Exact Reported	17 · Table 5 · Table 5
open-circuit voltage	1.2762	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D J-V simulation

NTU-9:1 · Model

Initial c-MOF HTL device parameters before optimisation.

Temperature: 300
Geometry: FTO/SnO2/SrZrS3/c-MOF/back contact
Context: model
Measurement source: 9 · 3.3. Influence of different c-MOFs as HTL · Fig. 5(c-h)

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	51.39	—	—	Visual Estimate Approximate	9 · 3.3. Influence of different c-MOFs as HTL · Fig. 5(c-h)
short-circuit current density	24.29	—	—	Visual Estimate Approximate	9 · 3.3. Influence of different c-MOFs as HTL · Fig. 5(c-h)
power conversion efficiency	11.34	—	—	Text Exact Reported	9 · 3.3. Influence of different c-MOFs as HTL · Fig. 5(c-h)
open-circuit voltage	0.9086	—	—	Visual Estimate Approximate	9 · 3.3. Influence of different c-MOFs as HTL · Fig. 5(c-h)

SCAPS-1D J-V simulation

NTU-9:22 · Model

Best optimized c-MOF HTL device selected from 193 simulated configurations.

Temperature: 300
Geometry: FTO/SnO2/SrZrS3/NTU-9/Ni
Context: model
Measurement source: 17 · Table 5 · Table 5

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	89.06	—	—	Table Exact Reported	17 · Table 5 · Table 5
short-circuit current density	25.76	—	—	Table Exact Reported	17 · Table 5 · Table 5
power conversion efficiency	29.78	—	—	Table Exact Reported	17 · Table 5 · Table 5
open-circuit voltage	1.3013	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D J-V simulation

Sr-MOF:1 · Model

Initial c-MOF HTL device parameters before optimisation.

Temperature: 300
Geometry: FTO/SnO2/SrZrS3/c-MOF/back contact
Context: model
Measurement source: 9 · 3.3. Influence of different c-MOFs as HTL · Fig. 5(c-h)

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	75.6	—	—	Visual Estimate Approximate	9 · 3.3. Influence of different c-MOFs as HTL · Fig. 5(c-h)
short-circuit current density	24.19	—	—	Visual Estimate Approximate	9 · 3.3. Influence of different c-MOFs as HTL · Fig. 5(c-h)
power conversion efficiency	13.17	—	—	Text Exact Reported	9 · 3.3. Influence of different c-MOFs as HTL · Fig. 5(c-h)
open-circuit voltage	0.72	—	—	Visual Estimate Approximate	9 · 3.3. Influence of different c-MOFs as HTL · Fig. 5(c-h)

SCAPS-1D J-V simulation

Sr-MOF:22 · Model

Best optimized c-MOF HTL device selected from 193 simulated configurations.

Temperature: 300
Geometry: FTO/SnO2/SrZrS3/Sr-MOF/Fe
Context: model
Measurement source: 17 · Table 5 · Table 5

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.53	—	—	Table Exact Reported	17 · Table 5 · Table 5
short-circuit current density	25.53	—	—	Table Exact Reported	17 · Table 5 · Table 5
power conversion efficiency	28.44	—	—	Table Exact Reported	17 · Table 5 · Table 5
open-circuit voltage	1.2583	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D C-F derived Nyquist plot

Cu3(HHTP)2:24 · Model

Optimized device recombination resistance from simulated Nyquist response.

Temperature: 300
Geometry: FTO/SnO2/SrZrS3/c-MOF/back contact
Context: model
Measurement source: 8 · 3.4. Nyquist plot measurements · Fig. 6

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
recombination resistanceMarked as a best value within this paper	1.70E+07	—	—	Text Rounded Reported	8 · 3.4. Nyquist plot measurements · Fig. 6

SCAPS-1D C-F derived Nyquist plot

Cu-MOF:75 · Model

Optimized device recombination resistance from simulated Nyquist response.

Temperature: 300
Geometry: FTO/SnO2/SrZrS3/c-MOF/back contact
Context: model
Measurement source: 8 · 3.4. Nyquist plot measurements · Fig. 6

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
recombination resistance	1.40E+07	—	—	Text Rounded Reported	8 · 3.4. Nyquist plot measurements · Fig. 6

SCAPS-1D C-F derived Nyquist plot

Fe2(DSBDC):21 · Model

Optimized device recombination resistance from simulated Nyquist response.

Temperature: 300
Geometry: FTO/SnO2/SrZrS3/c-MOF/back contact
Context: model
Measurement source: 8 · 3.4. Nyquist plot measurements · Fig. 6

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
recombination resistance	1.60E+07	—	—	Text Rounded Reported	8 · 3.4. Nyquist plot measurements · Fig. 6

SCAPS-1D C-F derived Nyquist plot

Mn2(DSBDC):22 · Model

Optimized device recombination resistance from simulated Nyquist response.

Temperature: 300
Geometry: FTO/SnO2/SrZrS3/c-MOF/back contact
Context: model
Measurement source: 8 · 3.4. Nyquist plot measurements · Fig. 6

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
recombination resistance	1.50E+07	—	—	Text Rounded Reported	8 · 3.4. Nyquist plot measurements · Fig. 6

SCAPS-1D C-F derived Nyquist plot

NTU-9:22 · Model

Optimized device recombination resistance from simulated Nyquist response.

Temperature: 300
Geometry: FTO/SnO2/SrZrS3/c-MOF/back contact
Context: model
Measurement source: 8 · 3.4. Nyquist plot measurements · Fig. 6

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
recombination resistance	6.20E+06	—	—	Text Rounded Reported	8 · 3.4. Nyquist plot measurements · Fig. 6

SCAPS-1D C-F derived Nyquist plot

Sr-MOF:22 · Model

Optimized device recombination resistance from simulated Nyquist response.

Temperature: 300
Geometry: FTO/SnO2/SrZrS3/c-MOF/back contact
Context: model
Measurement source: 8 · 3.4. Nyquist plot measurements · Fig. 6

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
recombination resistance	1.60E+07	—	—	Text Rounded Reported	8 · 3.4. Nyquist plot measurements · Fig. 6

SCAPS-1D Rs/Rsh/temperature sweep

Cu-MOF:75 · Model

Cu-MOF:75 parasitic resistance and temperature sensitivity simulated.

Temperature: 300-400
Context: model
Measurement source: 14-15 · 3.9. Impact of series resistance, shunt resistance, and operating temperature · Fig. 14

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
FF decline when Rs increases 1 to 10 Ω cm2	85.87 to 64.88	—	—	Text Range	14 · 3.9 · Fig. 14(a)
PCE decline when Rs increases 1 to 10 Ω cm2	29 to 22	—	—	Text Range	14 · 3.9 · Fig. 14(a)
recommended series resistanceMarked as a best value within this paper	1	—	—	Text Exact Reported	14 · 3.9 · Fig. 14(a)
Rsh sweep range	1000 to 5000	—	—	Text Range	14 · 3.9 · Fig. 14(b)
activation energy relative to absorber bandgap	Ea lower than 1.34 eV	—	—	Text Qualitative	15 · 3.9 · Fig. S1
PCE decline from 300 K to 400 K	30.60 to 28.4	—	—	Text Range	15 · 3.9 · Fig. 14(c)

SCAPS-1D QE simulation

Cu-MOF:75 · Model

Quantum efficiency response for initial and optimized devices; Cu-MOF response includes additional NIR absorption.

Temperature: 300
Context: model
Measurement source: 9 · 3.5. QE measurements · Fig. 7

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
Cu-MOF optimized NIR QE range	15 to 35	—	—	Text Range	9 · 3.5. QE measurements · Fig. 7
optimized devices spectral response plateau	100 % QE up to 850 nm	—	—	Text Rounded Reported	9 · 3.5. QE measurements · Fig. 7

SCAPS-1D supplementary parameter-sweep simulation

Cu3(HHTP)2:1 · Model

HTL 6 Optimization (Cu3(HHTP)2); varied HTL defect density = 10^12 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	80.81	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	21.50	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL defect density	10^12	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.0425	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu3(HHTP)2:10 · Model

HTL 6 Optimization (Cu3(HHTP)2); varied HTL electron affinity = 2.35 eV; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	81.45	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.51	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	22.70	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL electron affinity	2.35	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.0923	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu3(HHTP)2:11 · Model

HTL 6 Optimization (Cu3(HHTP)2); varied HTL electron affinity = 2.4 eV; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	82.05	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.51	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	23.91	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL electron affinity	2.4	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.1422	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu3(HHTP)2:12 · Model

HTL 6 Optimization (Cu3(HHTP)2); varied HTL electron affinity = 2.45 eV; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	82.63	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.51	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	25.12	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL electron affinity	2.45	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.1914	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu3(HHTP)2:13 · Model

HTL 6 Optimization (Cu3(HHTP)2); varied HTL electron affinity = 2.5 eV; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	83.15	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.51	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	26.30	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL electron affinity	2.5	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.2399	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu3(HHTP)2:14 · Model

HTL 6 Optimization (Cu3(HHTP)2); varied HTL carrier concentration = 10^14 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	83.15	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.51	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	26.30	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL carrier concentration	10^14	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.2399	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu3(HHTP)2:15 · Model

HTL 6 Optimization (Cu3(HHTP)2); varied HTL carrier concentration = 10^15 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	83.15	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.51	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	26.31	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL carrier concentration	10^15	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.2399	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu3(HHTP)2:16 · Model

HTL 6 Optimization (Cu3(HHTP)2); varied HTL carrier concentration = 10^16 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	83.15	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.51	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	26.31	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL carrier concentration	10^16	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.2399	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu3(HHTP)2:17 · Model

HTL 6 Optimization (Cu3(HHTP)2); varied HTL carrier concentration = 10^17 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	83.20	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.51	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	26.32	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL carrier concentration	10^17	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.2399	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu3(HHTP)2:18 · Model

HTL 6 Optimization (Cu3(HHTP)2); varied HTL carrier concentration = 10^18 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	83.88	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.51	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	26.54	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL carrier concentration	10^18	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.2402	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu3(HHTP)2:19 · Model

HTL 6 Optimization (Cu3(HHTP)2); varied HTL carrier concentration = 10^19 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	86.49	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.51	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	27.45	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL carrier concentration	10^19	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.2438	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu3(HHTP)2:2 · Model

HTL 6 Optimization (Cu3(HHTP)2); varied HTL defect density = 10^13 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	80.81	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	21.50	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL defect density	10^13	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.0425	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu3(HHTP)2:20 · Model

HTL 6 Optimization (Cu3(HHTP)2); varied HTL carrier concentration = 10^20 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.48	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.51	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	28.62	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL carrier concentration	10^20	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.2677	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu3(HHTP)2:21 · Model

HTL 6 Optimization (Cu3(HHTP)2); varied HTL thickness = 40 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.48	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.51	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	28.62	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL thickness	40	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.2677	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu3(HHTP)2:22 · Model

HTL 6 Optimization (Cu3(HHTP)2); varied HTL thickness = 80 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.48	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.51	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	28.62	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL thickness	80	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.2677	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu3(HHTP)2:23 · Model

HTL 6 Optimization (Cu3(HHTP)2); varied HTL thickness = 120 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.48	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.51	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	28.62	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL thickness	120	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.2677	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu3(HHTP)2:24 · Model

HTL 6 Optimization (Cu3(HHTP)2); varied HTL thickness = 160 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.48	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.51	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiencyMarked as a best value within this paper	28.62	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL thickness	160	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltageMarked as a best value within this paper	1.2677	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu3(HHTP)2:25 · Model

HTL 6 Optimization (Cu3(HHTP)2); varied HTL thickness = 200 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.48	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.51	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	28.62	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL thickness	200	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.2677	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu3(HHTP)2:3 · Model

HTL 6 Optimization (Cu3(HHTP)2); varied HTL defect density = 10^14 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	80.81	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	21.50	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL defect density	10^14	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.0425	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu3(HHTP)2:4 · Model

HTL 6 Optimization (Cu3(HHTP)2); varied HTL defect density = 10^15 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	80.81	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	21.50	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL defect density	10^15	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.0425	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu3(HHTP)2:5 · Model

HTL 6 Optimization (Cu3(HHTP)2); varied HTL defect density = 10^16 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	80.81	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	21.50	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL defect density	10^16	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.0425	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu3(HHTP)2:6 · Model

HTL 6 Optimization (Cu3(HHTP)2); varied HTL defect density = 10^17 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	80.81	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	21.50	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL defect density	10^17	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.0425	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu3(HHTP)2:7 · Model

HTL 6 Optimization (Cu3(HHTP)2); varied HTL defect density = 10^18 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	80.81	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	21.50	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL defect density	10^18	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.0425	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu3(HHTP)2:8 · Model

HTL 6 Optimization (Cu3(HHTP)2); varied HTL electron affinity = 2.25 eV; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	80.14	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	20.29	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL electron affinity	2.25	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	0.9924	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu3(HHTP)2:9 · Model

HTL 6 Optimization (Cu3(HHTP)2); varied HTL electron affinity = 2.3 eV; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	80.81	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	21.50	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL electron affinity	2.3	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.0425	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:1 · Model

ETL optimization (SnO2); varied ETL thickness = 10 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 1 · Supplementary information · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	55.78	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
short-circuit current density	23.35	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
power conversion efficiency	11.25	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
ETL thickness	10	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
open-circuit voltage	0.8639	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:10 · Model

ETL optimization (SnO2); varied ETL thickness = 100 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 1 · Supplementary information · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	55.80	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
short-circuit current density	23.30	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
power conversion efficiency	11.23	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
ETL thickness	100	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
open-circuit voltage	0.8639	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:11 · Model

ETL optimization (SnO2); varied ETL defect density = 10^12 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 1 · Supplementary information · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	55.80	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
short-circuit current density	23.34	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
power conversion efficiency	11.25	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
ETL defect density	10^12	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
open-circuit voltage	0.8640	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:12 · Model

ETL optimization (SnO2); varied ETL defect density = 10^13 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 1 · Supplementary information · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	55.80	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
short-circuit current density	23.34	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
power conversion efficiency	11.25	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
ETL defect density	10^13	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
open-circuit voltage	0.8640	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:13 · Model

ETL optimization (SnO2); varied ETL defect density = 10^14 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 1 · Supplementary information · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	55.80	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
short-circuit current density	23.34	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
power conversion efficiencyMarked as a best value within this paper	11.25	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
ETL defect density	10^14	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
open-circuit voltageMarked as a best value within this paper	0.8640	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:14 · Model

ETL optimization (SnO2); varied ETL defect density = 10^15 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 1 · Supplementary information · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	55.80	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
short-circuit current density	23.34	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
power conversion efficiency	11.25	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
ETL defect density	10^15	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
open-circuit voltage	0.8640	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:15 · Model

ETL optimization (SnO2); varied ETL defect density = 10^16 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 1 · Supplementary information · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	55.80	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
short-circuit current density	23.34	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
power conversion efficiency	11.25	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
ETL defect density	10^16	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
open-circuit voltage	0.8640	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:16 · Model

ETL optimization (SnO2); varied ETL defect density = 10^17 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 1 · Supplementary information · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	55.80	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
short-circuit current density	23.34	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
power conversion efficiency	11.25	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
ETL defect density	10^17	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
open-circuit voltage	0.8640	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:17 · Model

ETL optimization (SnO2); varied ETL defect density = 10^18 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 1 · Supplementary information · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	55.80	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
short-circuit current density	23.34	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
power conversion efficiency	11.25	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
ETL defect density	10^18	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
open-circuit voltage	0.8640	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:18 · Model

ETL optimization (SnO2); varied ETL carrier concentration = 10^12 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 1 · Supplementary information · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	55.56	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
short-circuit current density	23.36	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
power conversion efficiency	11.20	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
ETL carrier concentration	10^12	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
open-circuit voltage	0.8628	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:19 · Model

ETL optimization (SnO2); varied ETL carrier concentration = 10^13 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 1 · Supplementary information · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	55.56	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
short-circuit current density	23.36	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
power conversion efficiency	11.20	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
ETL carrier concentration	10^13	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
open-circuit voltage	0.8628	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:2 · Model

ETL optimization (SnO2); varied ETL thickness = 20 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 1 · Supplementary information · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	55.80	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
short-circuit current density	23.34	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
power conversion efficiencyMarked as a best value within this paper	11.25	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
ETL thickness	20	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
open-circuit voltageMarked as a best value within this paper	0.8640	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:20 · Model

ETL optimization (SnO2); varied ETL carrier concentration = 10^14 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 1 · Supplementary information · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	55.56	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
short-circuit current density	23.36	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
power conversion efficiency	11.20	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
ETL carrier concentration	10^14	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
open-circuit voltage	0.8628	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:21 · Model

ETL optimization (SnO2); varied ETL carrier concentration = 10^15 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 1 · Supplementary information · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	55.56	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
short-circuit current density	23.36	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
power conversion efficiency	11.20	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
ETL carrier concentration	10^15	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
open-circuit voltage	0.8628	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:22 · Model

ETL optimization (SnO2); varied ETL carrier concentration = 10^16 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 1 · Supplementary information · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	55.57	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
short-circuit current density	23.36	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
power conversion efficiency	11.20	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
ETL carrier concentration	10^16	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
open-circuit voltage	0.8628	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:23 · Model

ETL optimization (SnO2); varied ETL carrier concentration = 10^17 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 1 · Supplementary information · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	55.64	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
short-circuit current density	23.36	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
power conversion efficiency	11.22	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
ETL carrier concentration	10^17	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
open-circuit voltage	0.8632	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:24 · Model

ETL optimization (SnO2); varied ETL carrier concentration = 10^18 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 1 · Supplementary information · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	55.80	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
short-circuit current density	23.34	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
power conversion efficiencyMarked as a best value within this paper	11.25	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
ETL carrier concentration	10^18	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
open-circuit voltageMarked as a best value within this paper	0.8640	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:25 · Model

ETL optimization (SnO2); varied ETL carrier concentration = 10^19 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 1 · Supplementary information · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	55.85	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
short-circuit current density	23.31	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
power conversion efficiency	11.25	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
ETL carrier concentration	10^19	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
open-circuit voltage	0.8642	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:26 · Model

ETL optimization (SnO2); varied ETL carrier concentration = 10^20 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 1 · Supplementary information · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	55.87	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
short-circuit current density	23.31	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
power conversion efficiency	11.25	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
ETL carrier concentration	10^20	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
open-circuit voltage	0.8643	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:27 · Model

Absorber optimization (SrZrS3); varied absorber carrier concentration = 10^12 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 2 · Supplementary information · Table S2

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	55.78	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
short-circuit current density	23.34	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
power conversion efficiency	11.25	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
absorber carrier concentration	10^12	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
open-circuit voltage	0.8641	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:28 · Model

Absorber optimization (SrZrS3); varied absorber carrier concentration = 10^13 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 2 · Supplementary information · Table S2

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	55.79	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
short-circuit current density	23.34	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
power conversion efficiency	11.25	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
absorber carrier concentration	10^13	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
open-circuit voltage	0.8641	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:29 · Model

Absorber optimization (SrZrS3); varied absorber carrier concentration = 10^14 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 2 · Supplementary information · Table S2

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	55.80	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
short-circuit current density	23.34	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
power conversion efficiency	11.25	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
absorber carrier concentration	10^14	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
open-circuit voltage	0.8640	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:3 · Model

ETL optimization (SnO2); varied ETL thickness = 30 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 1 · Supplementary information · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	55.80	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
short-circuit current density	23.32	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
power conversion efficiency	11.24	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
ETL thickness	30	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
open-circuit voltage	0.8640	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:30 · Model

Absorber optimization (SrZrS3); varied absorber carrier concentration = 10^15 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 2 · Supplementary information · Table S2

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	56.00	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
short-circuit current density	23.34	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
power conversion efficiency	11.28	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
absorber carrier concentration	10^15	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
open-circuit voltage	0.8629	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:31 · Model

Absorber optimization (SrZrS3); varied absorber carrier concentration = 10^16 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 2 · Supplementary information · Table S2

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	61.69	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
short-circuit current density	23.35	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
power conversion efficiency	12.52	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
absorber carrier concentration	10^16	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
open-circuit voltage	0.8687	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:32 · Model

Absorber optimization (SrZrS3); varied absorber carrier concentration = 10^17 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 2 · Supplementary information · Table S2

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	73.51	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
short-circuit current density	20.29	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
power conversion efficiencyMarked as a best value within this paper	13.70	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
absorber carrier concentration	10^17	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
open-circuit voltage	0.9185	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:33 · Model

Absorber optimization (SrZrS3); varied absorber carrier concentration = 10^18 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 2 · Supplementary information · Table S2

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	81.22	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
short-circuit current density	14.98	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
power conversion efficiency	12.08	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
absorber carrier concentration	10^18	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
open-circuit voltage	0.9926	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:34 · Model

Absorber optimization (SrZrS3); varied absorber carrier concentration = 10^19 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 2 · Supplementary information · Table S2

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	65.11	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
short-circuit current density	13.61	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
power conversion efficiency	9.96	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
absorber carrier concentration	10^19	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
open-circuit voltage	1.1242	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:35 · Model

Absorber optimization (SrZrS3); varied absorber carrier concentration = 10^20 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 2 · Supplementary information · Table S2

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	57.20	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
short-circuit current density	6.26	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
power conversion efficiency	4.38	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
absorber carrier concentration	10^20	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
open-circuit voltage	1.2217	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:36 · Model

Absorber optimization (SrZrS3); varied absorber defect density = 10^12 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 2 · Supplementary information · Table S2

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	83.22	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
short-circuit current density	23.42	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
power conversion efficiencyMarked as a best value within this paper	18.28	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
absorber defect density	10^12	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
open-circuit voltage	0.9378	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:37 · Model

Absorber optimization (SrZrS3); varied absorber defect density = 10^13 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 2 · Supplementary information · Table S2

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	83.11	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
short-circuit current density	23.42	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
power conversion efficiency	18.25	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
absorber defect density	10^13	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
open-circuit voltage	0.9377	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:38 · Model

Absorber optimization (SrZrS3); varied absorber defect density = 10^14 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 2 · Supplementary information · Table S2

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	81.99	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
short-circuit current density	23.41	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
power conversion efficiency	17.97	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
absorber defect density	10^14	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
open-circuit voltage	0.9361	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:39 · Model

Absorber optimization (SrZrS3); varied absorber defect density = 10^15 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 2 · Supplementary information · Table S2

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	73.90	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
short-circuit current density	23.41	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
power conversion efficiency	15.98	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
absorber defect density	10^15	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
open-circuit voltage	0.9240	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:4 · Model

ETL optimization (SnO2); varied ETL thickness = 40 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 1 · Supplementary information · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	55.80	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
short-circuit current density	23.32	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
power conversion efficiency	11.24	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
ETL thickness	40	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
open-circuit voltage	0.8640	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:40 · Model

Absorber optimization (SrZrS3); varied absorber defect density = 10^16 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 2 · Supplementary information · Table S2

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	55.78	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
short-circuit current density	23.34	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
power conversion efficiency	11.25	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
absorber defect density	10^16	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
open-circuit voltage	0.8641	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:41 · Model

Absorber optimization (SrZrS3); varied absorber defect density = 10^17 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 2 · Supplementary information · Table S2

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	47.83	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
short-circuit current density	22.62	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
power conversion efficiency	9.21	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
absorber defect density	10^17	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
open-circuit voltage	0.8510	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:42 · Model

Absorber optimization (SrZrS3); varied absorber defect density = 10^18 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 2 · Supplementary information · Table S2

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	46.96	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
short-circuit current density	14.16	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
power conversion efficiency	5.96	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
absorber defect density	10^18	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
open-circuit voltage	0.8432	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:43 · Model

Absorber optimization (SrZrS3); varied absorber thickness = 100 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 2 · Supplementary information · Table S2

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	82.59	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
short-circuit current density	16.24	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
power conversion efficiency	12.41	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
absorber thickness	100	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
open-circuit voltage	0.9253	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:44 · Model

Absorber optimization (SrZrS3); varied absorber thickness = 200 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 2 · Supplementary information · Table S2

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	83.05	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
short-circuit current density	20.82	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
power conversion efficiency	16.15	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
absorber thickness	200	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
open-circuit voltage	0.9337	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:45 · Model

Absorber optimization (SrZrS3); varied absorber thickness = 300 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 2 · Supplementary information · Table S2

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	83.22	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
short-circuit current density	23.42	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
power conversion efficiency	18.28	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
absorber thickness	300	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
open-circuit voltage	0.9378	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:46 · Model

Absorber optimization (SrZrS3); varied absorber thickness = 400 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 2 · Supplementary information · Table S2

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	83.30	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
short-circuit current density	24.96	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
power conversion efficiency	19.55	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
absorber thickness	400	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
open-circuit voltage	0.9401	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:47 · Model

Absorber optimization (SrZrS3); varied absorber thickness = 500 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 2 · Supplementary information · Table S2

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	83.34	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
short-circuit current density	25.93	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
power conversion efficiency	20.34	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
absorber thickness	500	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
open-circuit voltage	0.9413	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:48 · Model

Absorber optimization (SrZrS3); varied absorber thickness = 600 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 2 · Supplementary information · Table S2

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	83.36	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
short-circuit current density	26.56	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
power conversion efficiencyMarked as a best value within this paper	20.86	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
absorber thickness	600	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
open-circuit voltage	0.9421	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:49 · Model

Absorber optimization (SrZrS3); varied absorber thickness = 700 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 2 · Supplementary information · Table S2

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	83.37	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
short-circuit current density	26.99	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
power conversion efficiency	21.21	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
absorber thickness	700	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
open-circuit voltage	0.9427	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:5 · Model

ETL optimization (SnO2); varied ETL thickness = 50 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 1 · Supplementary information · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	55.80	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
short-circuit current density	23.31	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
power conversion efficiency	11.24	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
ETL thickness	50	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
open-circuit voltage	0.8640	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:50 · Model

Absorber optimization (SrZrS3); varied absorber thickness = 800 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 2 · Supplementary information · Table S2

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	83.36	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
short-circuit current density	27.29	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
power conversion efficiency	21.46	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
absorber thickness	800	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
open-circuit voltage	0.9430	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:51 · Model

Absorber optimization (SrZrS3); varied absorber thickness = 900 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 2 · Supplementary information · Table S2

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	83.35	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
short-circuit current density	27.51	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
power conversion efficiency	21.63	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
absorber thickness	900	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
open-circuit voltage	0.9433	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:52 · Model

Absorber optimization (SrZrS3); varied absorber thickness = 1000 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 2 · Supplementary information · Table S2

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	83.33	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
short-circuit current density	27.67	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
power conversion efficiency	21.76	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
absorber thickness	1000	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2
open-circuit voltage	0.9435	—	—	SI Table Exact Reported	2 · Supplementary information · Table S2

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:53 · Model

HTL 1 Optimization (Cu-MOF); varied HTL defect density = 10^12 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	80.10	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	26.57	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	21.19	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL defect density	10^12	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	0.9957	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:54 · Model

HTL 1 Optimization (Cu-MOF); varied HTL defect density = 10^13 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	80.10	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	26.57	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	21.19	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL defect density	10^13	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	0.9957	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:55 · Model

HTL 1 Optimization (Cu-MOF); varied HTL defect density = 10^14 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	80.12	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	26.57	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	21.19	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL defect density	10^14	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	0.9955	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:56 · Model

HTL 1 Optimization (Cu-MOF); varied HTL defect density = 10^15 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	80.28	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	26.57	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	21.18	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL defect density	10^15	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	0.9933	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:57 · Model

HTL 1 Optimization (Cu-MOF); varied HTL defect density = 10^16 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	81.23	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	26.57	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	21.14	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL defect density	10^16	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	0.9798	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:58 · Model

HTL 1 Optimization (Cu-MOF); varied HTL defect density = 10^17 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	83.36	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	26.56	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	20.86	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL defect density	10^17	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	0.9421	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:59 · Model

HTL 1 Optimization (Cu-MOF); varied HTL defect density = 10^18 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	84.55	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	26.55	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	19.97	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL defect density	10^18	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	0.8896	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:6 · Model

ETL optimization (SnO2); varied ETL thickness = 60 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 1 · Supplementary information · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	55.80	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
short-circuit current density	23.31	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
power conversion efficiency	11.24	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
ETL thickness	60	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
open-circuit voltage	0.8639	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:60 · Model

HTL 1 Optimization (Cu-MOF); varied HTL electron affinity = 3.7 eV; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	80.10	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	26.57	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	21.19	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL electron affinity	3.7	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	0.9957	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:61 · Model

HTL 1 Optimization (Cu-MOF); varied HTL electron affinity = 3.75 eV; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	80.78	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	26.57	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	22.44	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL electron affinity	3.75	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	1.0457	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:62 · Model

HTL 1 Optimization (Cu-MOF); varied HTL electron affinity = 3.8 eV; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	81.42	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	26.56	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	23.69	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL electron affinity	3.8	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	1.0955	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:63 · Model

HTL 1 Optimization (Cu-MOF); varied HTL electron affinity = 3.85 eV; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	82.05	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	26.56	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	24.95	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL electron affinity	3.85	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	1.1447	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:64 · Model

HTL 1 Optimization (Cu-MOF); varied HTL carrier concentration = 10^14 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	82.05	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	26.56	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	24.95	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL carrier concentration	10^14	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	1.1447	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:65 · Model

HTL 1 Optimization (Cu-MOF); varied HTL carrier concentration = 10^15 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	82.05	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	26.56	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	24.95	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL carrier concentration	10^15	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	1.1447	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:66 · Model

HTL 1 Optimization (Cu-MOF); varied HTL carrier concentration = 10^16 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	82.05	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	26.56	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	24.95	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL carrier concentration	10^16	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	1.1447	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:67 · Model

HTL 1 Optimization (Cu-MOF); varied HTL carrier concentration = 10^17 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	82.01	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	26.56	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	24.94	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL carrier concentration	10^17	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	1.1446	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:68 · Model

HTL 1 Optimization (Cu-MOF); varied HTL carrier concentration = 10^18 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	82.45	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	26.56	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	25.06	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL carrier concentration	10^18	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	1.1442	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:69 · Model

HTL 1 Optimization (Cu-MOF); varied HTL carrier concentration = 10^19 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	85.67	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	26.56	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	26.05	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL carrier concentration	10^19	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	1.1447	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:7 · Model

ETL optimization (SnO2); varied ETL thickness = 70 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 1 · Supplementary information · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	55.80	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
short-circuit current density	23.31	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
power conversion efficiency	11.24	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
ETL thickness	70	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
open-circuit voltage	0.8639	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:70 · Model

HTL 1 Optimization (Cu-MOF); varied HTL carrier concentration = 10^20 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.43	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	26.56	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	27.45	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL carrier concentration	10^20	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	1.1684	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:71 · Model

HTL 1 Optimization (Cu-MOF); varied HTL thickness = 40 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.43	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	26.56	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	27.45	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL thickness	40	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	1.1684	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:72 · Model

HTL 1 Optimization (Cu-MOF); varied HTL thickness = 80 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.42	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	27.47	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	28.41	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL thickness	80	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	1.1696	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:73 · Model

HTL 1 Optimization (Cu-MOF); varied HTL thickness = 120 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.41	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	28.26	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	29.24	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL thickness	120	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	1.1705	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:74 · Model

HTL 1 Optimization (Cu-MOF); varied HTL thickness = 160 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.41	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	28.94	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	29.97	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL thickness	160	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	1.1713	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:75 · Model

HTL 1 Optimization (Cu-MOF); varied HTL thickness = 200 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.40	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	29.54	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiencyMarked as a best value within this paper	30.60	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL thickness	200	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltageMarked as a best value within this paper	1.1720	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:8 · Model

ETL optimization (SnO2); varied ETL thickness = 80 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 1 · Supplementary information · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	55.80	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
short-circuit current density	23.30	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
power conversion efficiency	11.23	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
ETL thickness	80	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
open-circuit voltage	0.8639	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1

SCAPS-1D supplementary parameter-sweep simulation

Cu-MOF:9 · Model

ETL optimization (SnO2); varied ETL thickness = 90 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 1 · Supplementary information · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	55.80	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
short-circuit current density	23.30	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
power conversion efficiency	11.23	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
ETL thickness	90	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1
open-circuit voltage	0.8639	—	—	SI Table Exact Reported	1 · Supplementary information · Table S1

SCAPS-1D supplementary parameter-sweep simulation

Fe2(DSBDC):1 · Model

HTL 3 Optimization (Fe2(DSBDC)); varied HTL defect density = 10^12 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	81.21	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.54	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	22.24	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL defect density	10^12	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.0723	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Fe2(DSBDC):10 · Model

HTL 3 Optimization (Fe2(DSBDC)); varied HTL electron affinity = 3.3 eV; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	82.41	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.54	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	24.66	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL electron affinity	3.3	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.1717	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Fe2(DSBDC):11 · Model

HTL 3 Optimization (Fe2(DSBDC)); varied HTL electron affinity = 3.35 eV; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	82.95	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.54	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	25.86	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL electron affinity	3.35	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.2207	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Fe2(DSBDC):12 · Model

HTL 3 Optimization (Fe2(DSBDC)); varied HTL carrier concentration = 10^14 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	82.95	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.54	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	25.86	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL carrier concentration	10^14	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.2207	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Fe2(DSBDC):13 · Model

HTL 3 Optimization (Fe2(DSBDC)); varied HTL carrier concentration = 10^15 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	82.95	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.54	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	25.86	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL carrier concentration	10^15	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.2207	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Fe2(DSBDC):14 · Model

HTL 3 Optimization (Fe2(DSBDC)); varied HTL carrier concentration = 10^16 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	82.96	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.54	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	25.87	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL carrier concentration	10^16	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.2207	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Fe2(DSBDC):15 · Model

HTL 3 Optimization (Fe2(DSBDC)); varied HTL carrier concentration = 10^17 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	83.01	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.54	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	25.88	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL carrier concentration	10^17	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.2207	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Fe2(DSBDC):16 · Model

HTL 3 Optimization (Fe2(DSBDC)); varied HTL carrier concentration = 10^18 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	83.72	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.54	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	26.11	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL carrier concentration	10^18	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.2211	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Fe2(DSBDC):17 · Model

HTL 3 Optimization (Fe2(DSBDC)); varied HTL carrier concentration = 10^19 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	86.33	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.54	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	27.01	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL carrier concentration	10^19	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.2251	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Fe2(DSBDC):18 · Model

HTL 3 Optimization (Fe2(DSBDC)); varied HTL carrier concentration = 10^20 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.50	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.54	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	28.23	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL carrier concentration	10^20	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.2491	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Fe2(DSBDC):19 · Model

HTL 3 Optimization (Fe2(DSBDC)); varied HTL thickness = 40 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.50	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.54	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	28.23	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL thickness	40	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.2491	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Fe2(DSBDC):2 · Model

HTL 3 Optimization (Fe2(DSBDC)); varied HTL defect density = 10^13 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	81.21	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.54	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	22.24	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL defect density	10^13	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.0723	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Fe2(DSBDC):20 · Model

HTL 3 Optimization (Fe2(DSBDC)); varied HTL thickness = 80 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.50	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.57	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	28.26	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL thickness	80	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.2491	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Fe2(DSBDC):21 · Model

HTL 3 Optimization (Fe2(DSBDC)); varied HTL thickness = 120 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.50	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.59	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiencyMarked as a best value within this paper	28.29	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL thickness	120	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.2491	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Fe2(DSBDC):22 · Model

HTL 3 Optimization (Fe2(DSBDC)); varied HTL thickness = 160 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.50	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.61	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	28.31	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL thickness	160	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.2491	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Fe2(DSBDC):23 · Model

HTL 3 Optimization (Fe2(DSBDC)); varied HTL thickness = 200 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.50	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.62	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	28.33	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL thickness	200	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.2492	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Fe2(DSBDC):3 · Model

HTL 3 Optimization (Fe2(DSBDC)); varied HTL defect density = 10^14 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	81.21	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.54	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	22.24	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL defect density	10^14	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.0723	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Fe2(DSBDC):4 · Model

HTL 3 Optimization (Fe2(DSBDC)); varied HTL defect density = 10^15 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	81.21	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.54	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	22.24	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL defect density	10^15	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.0723	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Fe2(DSBDC):5 · Model

HTL 3 Optimization (Fe2(DSBDC)); varied HTL defect density = 10^16 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	81.21	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.54	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	22.24	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL defect density	10^16	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.0723	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Fe2(DSBDC):6 · Model

HTL 3 Optimization (Fe2(DSBDC)); varied HTL defect density = 10^17 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	81.21	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.54	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	22.24	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL defect density	10^17	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.0723	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Fe2(DSBDC):7 · Model

HTL 3 Optimization (Fe2(DSBDC)); varied HTL defect density = 10^18 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	81.21	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.54	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	22.24	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL defect density	10^18	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.0723	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Fe2(DSBDC):8 · Model

HTL 3 Optimization (Fe2(DSBDC)); varied HTL electron affinity = 3.2 eV; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	81.21	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.54	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	22.24	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL electron affinity	3.2	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.0723	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Fe2(DSBDC):9 · Model

HTL 3 Optimization (Fe2(DSBDC)); varied HTL electron affinity = 3.25 eV; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	81.82	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.54	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	23.45	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL electron affinity	3.25	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.1222	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D temperature-dependent Voc simulation and linear fit

Cu-MOF:75 · Model

Cu-MOF:75 Voc plotted versus temperature; linear fit extrapolated to 0 K for activation-energy interpretation.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 6 · Supplementary information · Fig. S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
activation-energy interpretation from Voc-temperature plot	Ea lower than absorber bandgap	—	—	Caption Qualitative	6 · Supplementary information · Fig. S1

SCAPS-1D supplementary parameter-sweep simulation

Mn2(DSBDC):1 · Model

HTL 5 Optimization (Mn2(DSBDC)); varied HTL defect density = 10^12 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	80.94	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	21.72	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL defect density	10^12	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.0520	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Mn2(DSBDC):10 · Model

HTL 5 Optimization (Mn2(DSBDC)); varied HTL electron affinity = 2.6 eV; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	82.16	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	24.14	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL electron affinity	2.6	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.1516	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Mn2(DSBDC):11 · Model

HTL 5 Optimization (Mn2(DSBDC)); varied HTL electron affinity = 2.65 eV; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	82.71	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	25.35	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL electron affinity	2.65	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.2010	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Mn2(DSBDC):12 · Model

HTL 5 Optimization (Mn2(DSBDC)); varied HTL electron affinity = 2.7 eV; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	83.25	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	26.53	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL electron affinity	2.7	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.2488	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Mn2(DSBDC):13 · Model

HTL 5 Optimization (Mn2(DSBDC)); varied HTL carrier concentration = 10^14 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	83.25	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	26.53	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL carrier concentration	10^14	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.2488	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Mn2(DSBDC):14 · Model

HTL 5 Optimization (Mn2(DSBDC)); varied HTL carrier concentration = 10^15 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	83.25	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	26.53	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL carrier concentration	10^15	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.2488	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Mn2(DSBDC):15 · Model

HTL 5 Optimization (Mn2(DSBDC)); varied HTL carrier concentration = 10^16 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	83.25	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	26.53	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL carrier concentration	10^16	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.2488	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Mn2(DSBDC):16 · Model

HTL 5 Optimization (Mn2(DSBDC)); varied HTL carrier concentration = 10^17 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	83.28	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	26.54	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL carrier concentration	10^17	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.2488	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Mn2(DSBDC):17 · Model

HTL 5 Optimization (Mn2(DSBDC)); varied HTL carrier concentration = 10^18 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	83.95	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	26.75	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL carrier concentration	10^18	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.2489	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Mn2(DSBDC):18 · Model

HTL 5 Optimization (Mn2(DSBDC)); varied HTL carrier concentration = 10^19 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	86.57	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.51	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	27.66	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL carrier concentration	10^19	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.2521	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Mn2(DSBDC):19 · Model

HTL 5 Optimization (Mn2(DSBDC)); varied HTL carrier concentration = 10^20 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.45	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.51	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	28.80	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL carrier concentration	10^20	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.2762	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Mn2(DSBDC):2 · Model

HTL 5 Optimization (Mn2(DSBDC)); varied HTL defect density = 10^13 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	80.94	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	21.72	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL defect density	10^13	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.0520	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Mn2(DSBDC):20 · Model

HTL 5 Optimization (Mn2(DSBDC)); varied HTL thickness = 40 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.45	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.51	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	28.80	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL thickness	40	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.2762	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Mn2(DSBDC):21 · Model

HTL 5 Optimization (Mn2(DSBDC)); varied HTL thickness = 80 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.45	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	28.80	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL thickness	80	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.2762	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Mn2(DSBDC):22 · Model

HTL 5 Optimization (Mn2(DSBDC)); varied HTL thickness = 120 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.45	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiencyMarked as a best value within this paper	28.80	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL thickness	120	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltageMarked as a best value within this paper	1.2762	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Mn2(DSBDC):23 · Model

HTL 5 Optimization (Mn2(DSBDC)); varied HTL thickness = 160 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.45	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	28.80	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL thickness	160	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.2762	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Mn2(DSBDC):24 · Model

HTL 5 Optimization (Mn2(DSBDC)); varied HTL thickness = 200 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.45	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	28.80	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL thickness	200	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.2762	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Mn2(DSBDC):3 · Model

HTL 5 Optimization (Mn2(DSBDC)); varied HTL defect density = 10^14 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	80.94	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	21.72	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL defect density	10^14	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.0520	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Mn2(DSBDC):4 · Model

HTL 5 Optimization (Mn2(DSBDC)); varied HTL defect density = 10^15 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	80.94	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	21.72	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL defect density	10^15	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.0520	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Mn2(DSBDC):5 · Model

HTL 5 Optimization (Mn2(DSBDC)); varied HTL defect density = 10^16 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	80.94	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	21.72	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL defect density	10^16	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.0520	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Mn2(DSBDC):6 · Model

HTL 5 Optimization (Mn2(DSBDC)); varied HTL defect density = 10^17 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	80.94	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	21.72	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL defect density	10^17	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.0520	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Mn2(DSBDC):7 · Model

HTL 5 Optimization (Mn2(DSBDC)); varied HTL defect density = 10^18 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	80.94	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	21.72	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL defect density	10^18	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.0520	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Mn2(DSBDC):8 · Model

HTL 5 Optimization (Mn2(DSBDC)); varied HTL electron affinity = 2.5 eV; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	80.94	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	21.73	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL electron affinity	2.5	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.0520	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Mn2(DSBDC):9 · Model

HTL 5 Optimization (Mn2(DSBDC)); varied HTL electron affinity = 2.55 eV; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 5 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	81.55	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
power conversion efficiency	22.93	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
HTL electron affinity	2.55	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3
open-circuit voltage	1.1020	—	—	SI Table Exact Reported	5 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

NTU-9:1 · Model

HTL 2 Optimization (NTU-9); varied HTL defect density = 10^12 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	89.91	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	25.46	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	28.27	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL defect density	10^12	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	1.2350	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

NTU-9:10 · Model

HTL 2 Optimization (NTU-9); varied HTL electron affinity = 3.85 eV; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	89.41	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	24.69	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	26.25	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL electron affinity	3.85	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	1.1890	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

NTU-9:11 · Model

HTL 2 Optimization (NTU-9); varied HTL electron affinity = 3.9 eV; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.59	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	22.46	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	22.99	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL electron affinity	3.9	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	1.1551	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

NTU-9:12 · Model

HTL 2 Optimization (NTU-9); varied HTL carrier concentration = 10^14 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	87.48	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	25.55	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	28.99	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL carrier concentration	10^14	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	1.2971	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

NTU-9:13 · Model

HTL 2 Optimization (NTU-9); varied HTL carrier concentration = 10^15 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.10	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	25.57	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	29.24	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL carrier concentration	10^15	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	1.2979	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

NTU-9:14 · Model

HTL 2 Optimization (NTU-9); varied HTL carrier concentration = 10^16 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.42	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	25.58	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	29.37	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL carrier concentration	10^16	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	1.2986	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

NTU-9:15 · Model

HTL 2 Optimization (NTU-9); varied HTL carrier concentration = 10^17 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.64	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	25.59	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	29.47	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL carrier concentration	10^17	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	1.2993	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

NTU-9:16 · Model

HTL 2 Optimization (NTU-9); varied HTL carrier concentration = 10^18 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.81	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	25.59	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	29.55	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL carrier concentration	10^18	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	1.3000	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

NTU-9:17 · Model

HTL 2 Optimization (NTU-9); varied HTL carrier concentration = 10^19 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.95	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	25.59	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	29.61	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL carrier concentration	10^19	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	1.3006	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

NTU-9:18 · Model

HTL 2 Optimization (NTU-9); varied HTL carrier concentration = 10^20 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	89.06	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	25.60	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	29.66	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL carrier concentration	10^20	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	1.3011	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

NTU-9:19 · Model

HTL 2 Optimization (NTU-9); varied HTL thickness = 40 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	89.06	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	25.60	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	29.66	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL thickness	40	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	1.3011	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

NTU-9:2 · Model

HTL 2 Optimization (NTU-9); varied HTL defect density = 10^13 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.55	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	22.34	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	22.82	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL defect density	10^13	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	1.1540	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

NTU-9:20 · Model

HTL 2 Optimization (NTU-9); varied HTL thickness = 80 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	89.06	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	25.66	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	29.74	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL thickness	80	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	1.3012	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

NTU-9:21 · Model

HTL 2 Optimization (NTU-9); varied HTL thickness = 120 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	89.06	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	25.72	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	29.78	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL thickness	120	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	1.3013	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

NTU-9:22 · Model

HTL 2 Optimization (NTU-9); varied HTL thickness = 160 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	89.06	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	25.76	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiencyMarked as a best value within this paper	29.78	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL thickness	160	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltageMarked as a best value within this paper	1.3013	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

NTU-9:23 · Model

HTL 2 Optimization (NTU-9); varied HTL thickness = 200 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	89.06	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	25.80	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	29.78	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL thickness	200	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	1.3014	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

NTU-9:3 · Model

HTL 2 Optimization (NTU-9); varied HTL defect density = 10^14 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.39	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	21.77	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	22.11	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL defect density	10^14	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	1.1491	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

NTU-9:4 · Model

HTL 2 Optimization (NTU-9); varied HTL defect density = 10^15 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.31	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	21.54	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	21.82	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL defect density	10^15	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	1.1473	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

NTU-9:5 · Model

HTL 2 Optimization (NTU-9); varied HTL defect density = 10^16 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.27	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	21.41	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	21.66	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL defect density	10^16	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	1.1464	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

NTU-9:6 · Model

HTL 2 Optimization (NTU-9); varied HTL defect density = 10^17 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.25	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	21.32	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	21.56	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL defect density	10^17	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	1.1458	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

NTU-9:7 · Model

HTL 2 Optimization (NTU-9); varied HTL defect density = 10^18 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.23	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	21.27	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	21.49	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL defect density	10^18	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	1.1455	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

NTU-9:8 · Model

HTL 2 Optimization (NTU-9); varied HTL electron affinity = 3.75 eV; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	87.48	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	25.55	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	28.99	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL electron affinity	3.75	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	1.2971	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

NTU-9:9 · Model

HTL 2 Optimization (NTU-9); varied HTL electron affinity = 3.8 eV; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 3 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	89.91	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
short-circuit current density	25.46	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
power conversion efficiency	28.27	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
HTL electron affinity	3.8	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3
open-circuit voltage	1.2350	—	—	SI Table Exact Reported	3 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Sr-MOF:1 · Model

HTL 4 Optimization (Sr-MOF); varied HTL defect density = 10^12 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	81.93	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	23.68	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL defect density	10^12	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.1325	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Sr-MOF:10 · Model

HTL 4 Optimization (Sr-MOF); varied HTL electron affinity = 3.05 eV; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	82.50	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	24.89	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL electron affinity	3.05	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.1821	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Sr-MOF:11 · Model

HTL 4 Optimization (Sr-MOF); varied HTL electron affinity = 3.1 eV; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	83.05	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	26.08	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL electron affinity	3.1	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.2306	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Sr-MOF:12 · Model

HTL 4 Optimization (Sr-MOF); varied HTL carrier concentration = 10^14 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	83.06	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	26.08	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL carrier concentration	10^14	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.2306	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Sr-MOF:13 · Model

HTL 4 Optimization (Sr-MOF); varied HTL carrier concentration = 10^15 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	83.06	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	26.08	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL carrier concentration	10^15	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.2306	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Sr-MOF:14 · Model

HTL 4 Optimization (Sr-MOF); varied HTL carrier concentration = 10^16 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	83.06	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	26.08	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL carrier concentration	10^16	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.2306	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Sr-MOF:15 · Model

HTL 4 Optimization (Sr-MOF); varied HTL carrier concentration = 10^17 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	83.09	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	26.09	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL carrier concentration	10^17	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.2306	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Sr-MOF:16 · Model

HTL 4 Optimization (Sr-MOF); varied HTL carrier concentration = 10^18 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	83.76	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	26.31	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL carrier concentration	10^18	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.2307	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Sr-MOF:17 · Model

HTL 4 Optimization (Sr-MOF); varied HTL carrier concentration = 10^19 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	86.45	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	27.22	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL carrier concentration	10^19	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.2340	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Sr-MOF:18 · Model

HTL 4 Optimization (Sr-MOF); varied HTL carrier concentration = 10^20 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.53	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	28.43	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL carrier concentration	10^20	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.2583	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Sr-MOF:19 · Model

HTL 4 Optimization (Sr-MOF); varied HTL thickness = 40 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.53	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	28.43	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL thickness	40	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.2583	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Sr-MOF:2 · Model

HTL 4 Optimization (Sr-MOF); varied HTL defect density = 10^13 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	81.93	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	23.68	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL defect density	10^13	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.1325	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Sr-MOF:20 · Model

HTL 4 Optimization (Sr-MOF); varied HTL thickness = 80 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.53	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	28.43	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL thickness	80	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.2583	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Sr-MOF:21 · Model

HTL 4 Optimization (Sr-MOF); varied HTL thickness = 120 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.53	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.53	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	28.44	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL thickness	120	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.2583	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Sr-MOF:22 · Model

HTL 4 Optimization (Sr-MOF); varied HTL thickness = 160 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.53	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.53	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiencyMarked as a best value within this paper	28.44	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL thickness	160	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.2583	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Sr-MOF:23 · Model

HTL 4 Optimization (Sr-MOF); varied HTL thickness = 200 nm; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	88.53	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.54	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	28.45	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL thickness	200	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.2583	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Sr-MOF:3 · Model

HTL 4 Optimization (Sr-MOF); varied HTL defect density = 10^14 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	81.93	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	23.68	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL defect density	10^14	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.1325	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Sr-MOF:4 · Model

HTL 4 Optimization (Sr-MOF); varied HTL defect density = 10^15 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	81.92	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	23.68	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL defect density	10^15	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.1325	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Sr-MOF:5 · Model

HTL 4 Optimization (Sr-MOF); varied HTL defect density = 10^16 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	81.92	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	23.68	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL defect density	10^16	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.1325	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Sr-MOF:6 · Model

HTL 4 Optimization (Sr-MOF); varied HTL defect density = 10^17 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	81.92	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	23.68	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL defect density	10^17	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.1325	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Sr-MOF:7 · Model

HTL 4 Optimization (Sr-MOF); varied HTL defect density = 10^18 cm^-3; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	81.92	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	23.68	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL defect density	10^18	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.1325	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Sr-MOF:8 · Model

HTL 4 Optimization (Sr-MOF); varied HTL electron affinity = 2.95 eV; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	81.32	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	22.47	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL electron affinity	2.95	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.0828	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D supplementary parameter-sweep simulation

Sr-MOF:9 · Model

HTL 4 Optimization (Sr-MOF); varied HTL electron affinity = 3 eV; PV parameters reported in SI table.

Temperature: 300
Atmosphere: simulated AM1.5G; no experimental atmosphere
Geometry: SCAPS-1D FTO/SnO2/SrZrS3/c-MOF/back-contact superstrate model
Context: model system
Measurement source: 4 · Supplementary information · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
fill factor	81.93	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
short-circuit current density	25.52	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
power conversion efficiency	23.68	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
HTL electron affinity	3	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3
open-circuit voltage	1.1325	—	—	SI Table Exact Reported	4 · Supplementary information · Table S3

SCAPS-1D literature-derived input parameter set

SCAPS Cu3(HHTP)2 HTL material model · Model

Initial HTL layer parameters used in SCAPS-1D simulations; AM1.5G, 300 K for device simulations.

Temperature: 300
Geometry: FTO/SnO2/SrZrS3/c-MOF/back contact
Context: model
Measurement source: 3 · 2. Computation framework and device configuration · Table 1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
bandgap	2.85	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
acceptor concentration	0.0	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
effective density of states in conduction band	1.00E+20	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
donor concentration	1.00E+16	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
bulk defect density	1.00E+14	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
effective density of states in valence band	6.15E+20	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
electron affinity	2.8	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
initial HTL thickness	0.04	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
relative dielectric permittivity	9.6	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
hole mobility	0.8	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
electron mobility	1.00E+07	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1

SCAPS-1D literature-derived input parameter set

SCAPS Cu-MOF HTL material model · Model

Initial HTL layer parameters used in SCAPS-1D simulations; AM1.5G, 300 K for device simulations.

Temperature: 300
Geometry: FTO/SnO2/SrZrS3/c-MOF/back contact
Context: model
Measurement source: 3 · 2. Computation framework and device configuration · Table 1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
bandgap	1.34	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
acceptor concentration	0.0	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
effective density of states in conduction band	1.00E+18	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
donor concentration	1.00E+13	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
bulk defect density	1.00E+17	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
effective density of states in valence band	6.15E+18	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
electron affinity	4.0	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
initial HTL thickness	0.06	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
relative dielectric permittivity	9.2	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
hole mobility	1.00E+07	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
electron mobility	1.00E+07	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1

SCAPS-1D literature-derived input parameter set

SCAPS Fe2(DSBDC) HTL material model · Model

Initial HTL layer parameters used in SCAPS-1D simulations; AM1.5G, 300 K for device simulations.

Temperature: 300
Geometry: FTO/SnO2/SrZrS3/c-MOF/back contact
Context: model
Measurement source: 3 · 2. Computation framework and device configuration · Table 1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
bandgap	1.92	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
acceptor concentration	0.0	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
effective density of states in conduction band	1.00E+18	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
donor concentration	1.00E+14	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
bulk defect density	1.00E+16	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
effective density of states in valence band	6.15E+19	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
electron affinity	3.6	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
initial HTL thickness	0.06	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
relative dielectric permittivity	9.0	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
hole mobility	800.0	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
electron mobility	1.00E+07	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1

SCAPS-1D literature-derived input parameter set

SCAPS Mn2(DSBDC) HTL material model · Model

Initial HTL layer parameters used in SCAPS-1D simulations; AM1.5G, 300 K for device simulations.

Temperature: 300
Geometry: FTO/SnO2/SrZrS3/c-MOF/back contact
Context: model
Measurement source: 3 · 2. Computation framework and device configuration · Table 1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
bandgap	2.6	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
acceptor concentration	0.0	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
effective density of states in conduction band	1.80E+18	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
donor concentration	1.00E+14	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
bulk defect density	1.00E+15	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
effective density of states in valence band	9.15E+19	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
electron affinity	2.5	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
initial HTL thickness	0.07	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
relative dielectric permittivity	10.0	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
hole mobility	100.0	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
electron mobility	1.00E+07	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1

SCAPS-1D literature-derived input parameter set

SCAPS NTU-9 HTL material model · Model

Initial HTL layer parameters used in SCAPS-1D simulations; AM1.5G, 300 K for device simulations.

Temperature: 300
Geometry: FTO/SnO2/SrZrS3/c-MOF/back contact
Context: model
Measurement source: 3 · 2. Computation framework and device configuration · Table 1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
bandgap	1.72	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
acceptor concentration	0.0	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
effective density of states in conduction band	1.00E+20	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
donor concentration	1.00E+16	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
bulk defect density	1.00E+15	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
effective density of states in valence band	6.15E+20	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
electron affinity	3.8	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
initial HTL thickness	0.04	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
relative dielectric permittivity	8.0	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
hole mobility	2.00E+04	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
electron mobility	50.0	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1

SCAPS-1D literature-derived input parameter set

SCAPS Sr-MOF HTL material model · Model

Initial HTL layer parameters used in SCAPS-1D simulations; AM1.5G, 300 K for device simulations.

Temperature: 300
Geometry: FTO/SnO2/SrZrS3/c-MOF/back contact
Context: model
Measurement source: 3 · 2. Computation framework and device configuration · Table 1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
bandgap	2.3	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
acceptor concentration	0.0	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
effective density of states in conduction band	1.00E+20	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
donor concentration	1.00E+15	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
bulk defect density	1.00E+14	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
effective density of states in valence band	6.15E+21	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
electron affinity	3.4	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
initial HTL thickness	0.04	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
relative dielectric permittivity	9.8	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
hole mobility	100.0	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1
electron mobility	1.00E+07	—	—	Table Exact Reported	3 · 2. Computation framework and device configuration · Table 1