Computational Modelling — Hydrogenic Defects in Ferromagnetic Cu3(HITP)2 (HITP ≡ 2,3,6,7,10,11-Hexaiminotriphenylene), a 2D Metal-Organic Framework

11 measurement groups · 24 results

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

Bader charge analysis and optimised local structure comparison.

Cu3(HITP)2 with neutral interstitial H* · Model

N-donor Bader charges and Cu-N bond lengths read from Figure 3 for single interstitial H charge states q = 0, +1 and -1; pristine no-H reference reported in caption.

Atmosphere: not_applicable
Geometry: local defect environment in monolayer model
Context: defective model with pristine reference
Measurement source: main p.4, article p.2701 · Results and discussion · Figure 3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
H- interstitial N-site Bader charges	1.28, 1.34, 1.34, 1.28 e	—	—	Figure Axis Exact Reported	main p.4, article p.2701 · Figure 3 · Figure 3c
*Single H interstitial N-site Bader charges**	1.24, 1.31, 1.33, 1.29 e	—	—	Figure Axis Exact Reported	main p.4, article p.2701 · Figure 3 · Figure 3a
H+ interstitial N-site Bader charges	1.27, 1.32, 1.29, 1.29 e	—	—	Figure Axis Exact Reported	main p.4, article p.2701 · Figure 3 · Figure 3b
Pristine N-site Bader charge	1.29 for all N sites	1.29 e	—	Caption Exact Reported	main p.4, article p.2701 · Figure caption · Figure 3

HSEsol electronic band-structure calculation.

Cu3(HITP)2 with two neutral interstitial H* defects · Model

Defective monolayer Cu3(HITP)2 containing 2H* interstitials.

Atmosphere: not_applicable
Geometry: periodic monolayer model
Context: defective model
Measurement source: main p.3, article p.2700 · Results and discussion · Figure 2d

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
*Band gap of Cu3(HITP)2 with 2H interstitials**Marked as a best value within this paper	0.71 eV	0.71 eV	—	Caption Exact Reported	main p.3, article p.2700 · Figure caption; Results and discussion · Figure 2d

HSEsol electronic band-structure calculation.

Cu3(HITP)2 with interstitial H- · Model

Single H- interstitial in Cu3(HITP)2.

Atmosphere: not_applicable
Geometry: periodic monolayer model
Context: defective model
Measurement source: main p.4, article p.2701 · Results and discussion · Figure 3c

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
Band gap of Cu3(HITP)2 with H- interstitial	0.4 eV	0.4 eV	—	Text Rounded Reported	main p.4, article p.2701 · Results and discussion · Figure 3c

HSEsol electronic band-structure calculation.

Cu3(HITP)2 with neutral interstitial H* · Model

Single neutral H* interstitial in Cu3(HITP)2.

Atmosphere: not_applicable
Geometry: periodic monolayer model
Context: defective model
Measurement source: main p.3-4, article pp.2700-2701 · Results and discussion · Figure 3a

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
*Band gap of Cu3(HITP)2 with single neutral H interstitial**	0.27 eV at the M point	0.27 eV	—	Text Exact Reported	main p.3-4, article pp.2700-2701 · Results and discussion · Figure 3a

HSEsol electronic band-structure calculation.

Cu3(HITP)2 with interstitial H+ · Model

Single H+ interstitial in Cu3(HITP)2.

Atmosphere: not_applicable
Geometry: periodic monolayer model
Context: defective model
Measurement source: main p.4, article p.2701 · Results and discussion · Figure 3b

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
Band gap of Cu3(HITP)2 with H+ interstitial	0.26 eV	0.26 eV	—	Text Exact Reported	main p.4, article p.2701 · Results and discussion · Figure 3b

HSEsol electronic band-structure calculation.

Pristine monolayer Cu3(HITP)2 computational cell · Model

Band structure sampled along Gamma, M and K k-vectors of the irreducible Brillouin zone.

Atmosphere: not_applicable
Geometry: periodic monolayer model
Context: pristine model
Measurement source: main p.2, article p.2699 · Results and discussion · Figure 1c,d

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
Pristine Cu3(HITP)2 monolayer band gapMarked as a best value within this paper	0.39 eV	0.39 eV	—	Text Exact Reported	main p.2, article p.2699 · Results and discussion · Figure 1
Cu-centred occupied d bands relative to Fermi level	-4 eV from EF	-4 eV	—	Text Rounded Reported	main p.2, article p.2699 · Results and discussion · Figure 1d
Unoccupied Cu d state above Fermi level	~2 eV above the Fermi level	2 eV	—	Text Approximate	main p.3, article p.2700 · Results and discussion · Figure 1

Charged-defect formation-energy calculation with FNV finite-size correction.

Cu3(HITP)2 with two neutral interstitial H* defects · Model

Two neutral interstitial hydrogen atoms, one per linker, compared under hydrogen-rich and hydrogen-poor limits.

Atmosphere: not_applicable
Geometry: periodic monolayer point-defect model
Context: defective model
Measurement source: main p.3, article p.2700 · Results and discussion · Figure 2

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
*Approximate 2H formation energy under H-poor conditions**Marked as a best value within this paper	approximately -0.85 eV from Figure 2c	-0.85 eV	visual estimate from axis	Figure Axis Approximate	main p.3, article p.2700 · Results and discussion · Figure 2c
*Approximate 2H formation energy under H-rich conditions**Marked as a best value within this paper	approximately -1.85 eV from Figure 2b	-1.85 eV	visual estimate from axis	Figure Axis Approximate	main p.3, article p.2700 · Results and discussion · Figure 2b
*2H interstitial relative favourability**Marked as a best value within this paper	most negative formation energies	—	—	Text Qualitative	main p.3, article p.2700 · Results and discussion · Figure 2

Charged-defect formation-energy calculation with FNV finite-size correction.

Cu3(HITP)2 with neutral interstitial H* · Model

Single interstitial hydrogen charge states H+, H* and H- under hydrogen-rich and hydrogen-poor conditions; chemical potentials from ref. 26.

Atmosphere: not_applicable
Geometry: periodic monolayer point-defect model
Context: defective model
Measurement source: main p.3, article p.2700 · Results and discussion · Figure 2b,c

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
Single interstitial hydrogen formation energies	very low for all charge states	—	—	Text Qualitative	main p.3, article p.2700 · Results and discussion · Figure 2b,c
Approximate neutral Hi formation energy under H-poor conditions	approximately -0.4 eV from Figure 2c plateau	-0.4 eV	visual estimate from axis	Figure Axis Approximate	main p.3, article p.2700 · Results and discussion · Figure 2c
Approximate neutral Hi formation energy under H-rich conditions	approximately -1.1 eV from Figure 2b plateau	-1.1 eV	visual estimate from axis	Figure Axis Approximate	main p.3, article p.2700 · Results and discussion · Figure 2b

Charged-defect formation-energy calculation with FNV finite-size correction.

Hydrogen-vacancy Cu3(HITP)2 model · Model

Hydrogen-vacancy charge states q = -1, 0 and +1 under hydrogen-rich and hydrogen-poor conditions; chemical potentials from ref. 26.

Atmosphere: not_applicable
Geometry: periodic monolayer point-defect model
Context: defective model
Measurement source: main p.2-3, article pp.2699-2700 · Computational details; Results and discussion · Figure 2b,c

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
Hydrogen vacancy q = -1 formation energy range	~2.5 to 3.0 eV	—	range 2.5-3.0 eV	Text Range	main p.3, article p.2700 · Results and discussion · Figure 2b,c
Neutral hydrogen vacancy formation energy range	Ef = 1.6-2 eV	—	range 1.6-2 eV	Text Range	main p.3, article p.2700 · Results and discussion · Figure 2b,c

Spin-polarised DFT in VASP; PAW; HSEsol/HSE06 with PBEsol; geometry optimisation and electronic structure.

Density functional theory

Pristine monolayer Cu3(HITP)2 computational cell · Model

Plane-wave cutoff 500 eV; Gamma-centred 2 x 2 x 1 k-point mesh; 20 Angstrom z-direction vacuum; force convergence <0.01 eV/Angstrom; final energy change <1e-6 eV per atom.

Atmosphere: not_applicable
Geometry: periodic monolayer supercell
Context: pristine model host
Measurement source: main p.2, article p.2699 · Computational details

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
Plane-wave kinetic energy cutoff	500 eV	500 eV	—	Text Exact Reported	main p.2, article p.2699 · Computational details
Geometry-optimisation force convergence threshold	<0.01 eV/Angstrom	0.01 eV/Angstrom	—	Text Exact Reported	main p.2, article p.2699 · Computational details
Vacuum spacing perpendicular to layer	20 Angstrom	20 Angstrom	—	Text Exact Reported	main p.2, article p.2699 · Computational details

2 x 2 supercell magnetic-ordering comparison.

Pristine monolayer Cu3(HITP)2 computational cell · Model

Ferromagnetic and antiferromagnetic d-electron configurations compared before enforcing ferromagnetic order in the three-Cu unit cell.

Atmosphere: not_applicable
Geometry: 2 x 2 monolayer supercell
Context: pristine model
Measurement source: main p.3, article p.2700 · Results and discussion

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
Ferromagnetic ordering favourability with interstitial H charge states	0.01 eV	0.01 eV	—	Text Exact Reported	main p.3, article p.2700 · Results and discussion
Ferromagnetic stabilisation relative to antiferromagnetic analogueMarked as a best value within this paper	0.01 eV more stable	0.01 eV	—	Text Exact Reported	main p.3, article p.2700 · Results and discussion