Computational Modelling

DFT band-structure calculation using VASP with PBE, DFT-D3 and Hubbard U=3 eV on Cu

DFT model of bulk AA-stacked Cu3(HFcHBC)2 · Model

Experimentally resolved crystal structure geometry optimised; cutoff 520 eV; PBE exchange-correlation; DFT-D3; U correction on Cu.

Context: model
Measurement source: 4-5 · Modeling and electronic structure · Figure 3; Figure S24

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
bulk conduction-band dispersion across Fermi level	about 0.2 eV	—	—	Text Approximate	5 · Electronic band structure · Figure 3c
monolayer DFT metallic behaviour	bands widely dispersed across the Fermi level; intrinsic metallic behaviour	—	—	Qualitative Qualitative	5 · Electronic band structure · Figure 3b

DFT model of monolayer Cu3(HFcHBC)2 · Model

Optimized molecular structures of TP, TN, cHBC and HFcHBC; CuO4 linker levels also compared in Figure 1/S1.

Context: model
Measurement source: 4 · Modeling and electronic structure · Figure S1; Figure 1a

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
cHBC LUMO energy	-1.941 eV	—	—	Text Exact Reported	4 · Results and Discussion · Figure 1a; Figure S1
CN LUMO energy	-1.607 eV	—	—	Text Exact Reported	4 · Results and Discussion · Figure 1a; Figure S1
FcHBC LUMO energy	-2.295 eV	—	—	Text Exact Reported	4 · Results and Discussion · Figure 1a; Figure S1
TN LUMO energy	-1.852 eV	—	—	Text Exact Reported	4 · Results and Discussion · Figure 1a; Figure S1
TP LUMO energy	-1.137 eV	—	—	Text Exact Reported	4 · Results and Discussion · Figure 1a; Figure S1