Computational Modelling

DFT+U using VASP 5.4.1; PBE GGA; PAW; Grimme-D2; Bader analysis; BoltzTraP2

Cu2[PcCu-O8] multilayer AA-inclined DFT model · Model

Plane-wave cutoff 400 eV; EDIFF 1E-6 eV; U = 4 eV and J = 1 eV for Cu d orbitals; monolayer k grids 3x3x1 optimisation and 9x9x1 band; 3D stack k grids 2x2x4 optimisation and 4x4x6 band; BoltzTraP2 interpolation onto 7-times denser grid

Geometry: Monolayer and 3D stacked periodic models
Context: Computational model systems
Measurement source: SI p. 5 · Modeling and electronic structure · Figure 4; Table S2

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
Calculated conductivity anisotropy trend	Intralayer conductivity much lower than interlayer conductivity	—	—	Qualitative Qualitative	p. 6 · Theoretical Calculation of Electronic Structures · Figure 4c
DFT interlayer-direction band dispersion	0.19 eV along Gamma-Z	—	—	Text Exact Reported	p. 6 · Theoretical Calculation of Electronic Structures · Figure 4b
DFT monolayer bandgap	about 0.35 eV	—	—	Text Approximate	p. 6 · Theoretical Calculation of Electronic Structures · Figure 4a
DFT AA-inclined multilayer bandgap	0.03 eV	—	—	Text Exact Reported	p. 6 · Theoretical Calculation of Electronic Structures · Figure 4b
PBE-D2 optimised monolayer lattice parameter	a = b = 18.36 A	1.836 nm	—	Text Exact Reported	SI p. 5 · Modeling and electronic structure
SCAN optimised monolayer lattice parameter	a = b = 18.40 A	1.84 nm	—	Text Exact Reported	SI p. 5 · Modeling and electronic structure

1 measurement group · 6 results