Microscopy Morphology

AFM topography and statistical grain/roughness analysis

Cu3(HHTP)2-xC spray LBL-LPE thin-film growth-cycle series, x = 1-60 · Thin Film

Bruker Dimension ICON AFM, ScanAsyst in air mode; cantilever spring constant 0.4 N/m; setpoint 0.02 +/- 0.005 V; scan rate 1 Hz; 256 lines.

Atmosphere: air
Geometry: 500 nm x 500 nm AFM images in Figures 1 and S4; cross-sectional AFM in Figure S5
Context: pristine Cu3(HHTP)2-xC growth-cycle series
Measurement source: p003 · 1.1 Materials and General Methods · Figures 1, 2a-b, S4, S5

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
Cu3(HHTP)2-1C average roughness Ra	approximately 0.7 nm	7e-10 m	approximately	Text Approximate	p003 · Results and Discussion · Figure 1b; Figure 2a
Cu3(HHTP)2-2C average roughness Ra	2.47 nm	2.47e-9 m	—	Text Exact Reported	p003 · Results and Discussion · Figure 1c; Figure 2a
surface grain transverse diameter during growth	most grain size < 40 nm; surface grain restricted to < 40 nm in each cycle	4e-8 m	upper-bound descriptor	Text Approximate	p002-p003 · Results and Discussion · Figure 1; Figure 2b
Cu3(HHTP)2-xC roughness for x = 4-20	approximately 2.2 nm with little fluctuation	2.2e-9 m	approximately	Text Approximate	p003 · Results and Discussion · Figure 2a
blank substrate average roughness Ra	0.3 nm	3e-10 m	—	Text Rounded Reported	p003 · Results and Discussion · Figure 2a
Cu3(HHTP)2-1C thickness from S5 labels	labels 2.06, 2.01, 2.27, 2.42 and 2.15 nm; average about 2.18 nm	2.18e-9 m	spread across five labelled line profiles	Visual Estimate Approximate	p008 · 2. Figures · Figure S5
Cu3(HHTP)2-20C thickness from S5 labels	labels 38.0, 38.8, 38.2, 38.5 and 38.3 nm; average about 38.4 nm	3.84e-8 m	spread across five labelled line profiles	Visual Estimate Approximate	p008 · 2. Figures · Figure S5
homogeneous thickness growth rate	approximately 2 nm per cycle	—	approximately	Text Approximate	p003 · Results and Discussion · Figure 2a; Figure S5

Cu3(HHTP)2-xC spray LBL-LPE thin-film growth-cycle series, x = 1-60 · Thin Film

Zeiss Sigma 300 field-emission SEM at 3 kV; cross-sectional views for x = 10, 20, 30 and 50 in SI.

Geometry: thin-film cross sections; Figure 2c shows 20C, Figure S7 shows 10C/20C/30C/50C
Context: pristine Cu3(HHTP)2-xC thin films
Measurement source: p003 · 1.1 Materials and General Methods · Figure 2c; Figure S7

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
cross-sectional morphology	dense bottom and rough top profile; dense-bottom proportion increases with growth cycle	—	—	Text Qualitative	p003 · Results and Discussion · Figure 2c; Figure S7

Cu3(HHTP)2-30C peeled-film TEM slice · Thin Film

FEI TALOS F200X G2 field-emission TEM at 200 kV and 200 pm electron beam current; beam perpendicular to peeled slices.

Geometry: peeled Cu3(HHTP)2-30C thin-film slices; thicker rough top and thinner smooth bottom regions
Context: pristine 30-cycle Cu3(HHTP)2 film
Measurement source: p004 · Results and Discussion · Figure 3d-f; Figures S11-S12

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
30C thinner slice bottom-region orientation	bright FFT diffraction points divided into a few hexagonal lattice point sets; bottom part has preferred orientation in the ab plane and fused mesocrystal structure	—	—	Text Qualitative	p004 · Results and Discussion · Figure 3e-f; Figure S12
30C thicker slice top-region FFT assignment	diffraction cycles/rings of (hk0); none of (00l) found; polycrystal nature and oriented growth along (00l) direction	—	—	Text Qualitative	p004 · Results and Discussion · Figure 3d; Figure S11