First-Principles Insights into the Electronic Structure, Optical and Band Alignment Properties of Earth-Abundant Cu2SrSnS4 Solar Absorber - data

Cu2SrSnS4 (CSTS) is a promising alternative candidate to Cu2ZnSnS4 (CZTS) for single- or multi-junction photovoltaics (PVs) owing to its efficient light-absorbing capability, earth-abundant, nontoxic constituents, and suitable defect properties. However, as a novel absorber material, several fundamental properties need to be characterized before further progress can be made in CSTS photovoltaics. In this letter, hybrid density functional theory (DFT) calculations have been used to comprehensively characterize for the first time, the electronic structure, band alignment, and optical properties of CSTS. It is demonstrated that CSTS possesses the ideal electronic structure (direct band gap of 1.98 eV and small photocarrier effective masses) and optical properties (high extinction coefficient and wide absorption) suitable for photovoltaic applications. Simulated X-ray photoelectron spectroscopy (XPS) valence band spectra using variable excitation energies show that Cu-3d electronic state dominates the valence band maximum of CSTS. Furthermore, the vacuum-aligned band diagram between CSTS and other common absorbers (CZTS, CIGS, CdTe) and the common n-type partner materials (CdS, ZnO) was constructed, which indicate staggered type-II band alignment at the CSTS/CdS and CSTS/ZnO interfaces. Based on these results, interface band offset engineering and alternative device architectures are suggested to improve charge carrier separation and power conversion efficiencies of CSTS. Data underpinning the work are available in the .xlsx format (can be viewed either by MS Office or Libre Office) comprising 13 datasheets named according to their contents. Data for optimized bulk structure and surfaces models are available in CONTCAR format of the VASP simulation program and can be visualized using the VESTA software. The simulated powder diffraction pattern, band structure along high-symmetry directions, projected electronic density of states (PDOS), optical properties data, and simulated valence band edge spectra of Cu2SrSnS4 at Al Kα1 (hν=1.486 keV), hν=4.068 keV and hν = 8.133 keV are provided.