Cu2ZnSnS4 as a potential photovoltaic material: A hybrid Hartree-Fock density functional theory study

Author(s)
Joachim Paier, Ryoji Asahi, Akihiro Nagoya, Georg Kresse
Abstract

First-principles calculations for the potential photovoltaic material Cu2ZnSnS4 (CZTS) are presented using density functional theory and the Perdew-Burke-Ernzerhof exchange-correlation functional as well as using the Heyd-Scuseria-Ernzerhof (HSE) hybrid functional. The HSE results compare very favorably to experimental data for the lattice constants and the band gap, as demonstrated for CZTS and selected ternary chalcopyrites such as CuInS2, CuInSe2, CuGaS2, and CuGaSe2. Furthermore the HSE band structure is validated using G0W0 quasiparticle calculations. The valence band is found to be made up by an antibonding linear combination of Cu-3d states and S-3p states, whereas an isolated band made up by Sn-5s and S-3p states dominates the conduction band. In the visible wavelength, the optical properties are determined by transitions from the Cu-3d/S-3p states into this conduction band. Comparison of the optical spectra calculated in the independent-particle approximation and using time-dependent hybrid functional theory indicates very small excitonic effects. For the structural properties, the kesterite-type structure of I4¯ symmetry is predicted to be the most stable one, possibly along with cation disorder within the Cu-Zn layer. The energy differences between structural modifications are well approximated by a simple ionic model.

Organisation(s)
Computational Materials Physics
External organisation(s)
Toyota Central R&D Labs., Inc.
Journal
Physical Review B
Volume
79
No. of pages
8
ISSN
1098-0121
DOI
https://doi.org/10.1103/PhysRevB.79.115126
Publication date
2009
Peer reviewed
Yes
Austrian Fields of Science 2012
1030 Physics, Astronomy
Sustainable Development Goals
SDG 7 - Affordable and Clean Energy
Portal url
https://ucrisportal.univie.ac.at/en/publications/cu2znsns4-as-a-potential-photovoltaic-material-a-hybrid-hartreefock-density-functional-theory-study(13c62f0a-74ab-4fe3-b72f-b6d87a311d1b).html