Anisotropic optical properties of Cu2ZnSn(SxSe1−x)4 solid solutions: First-principles calculations with TB-mBJ+U

Abstract

The main aim of this work is to determine and explain the relationships between optoelectronic properties and the sulfur anion content in Cu2ZnSn(SxSe1−x)4 solid solution. Band gap and absorption coefficient are of primary interest to the engineers and scientists researcher worked in optoelectronic field. Herein, the electronic and optical properties are calculated based on 128 conventional atoms within lattice parameters obtained at 300 K by using the FP-LAPW method combined with quasi-harmonic Debye model. The composition dependent band gaps of CZTSSe solid solutions are investigated by TB-mBJ+U. As results, all materials are semiconductors with a direct band gap ranging from 0.614 to 0.99 eV. The band gap variation increases as a function of sulfur anion content and showed a positive deviation from Vegard's law with a very small downward bowing parameter of + 0.079 eV. The density of state (DOS) calculations indicate that the energy bands of VBM involve Cu_d/anion(S/Se)_p hybridized antibonding-like states. Based on band alignment, the Ec offset between CZTS and CZTSe is larger than the Ev offset. These results are reported previously in other work and are confirmed in this study. Our work included a systematic comparison of the influence of S/(S+Se) atomic ratios on optical quantities. The dielectric function tensors show remarkable anisotropy. In addition, the static dielectric constants are found to decrease with sulfur anion content. The CZTSSe is proved to be suitable for good solar cells with high absorption coefficient (> 104 cm−1). Such deep optical studies would be helpful for future optoelectronic applications of these compounds with different S/(S+Se) atomic ratios.