Constructing density functional tight-binding parameters for electronic structure modeling of lead-bromide perovskites, perovskitoids, and related structures
Abstract
Density functional tight-binding (DFTB), a semi-empirical approach rooted in density functional theory, is well-suited for simulating large periodic systems. Following Jiang et al. [Phys. Rev. Mater. 9, 023803 (2025)], we have specifically tailored DFTB parameters for accurate electronic bandgap calculations in both three-dimensional and two-dimensional lead bromide perovskites, significantly reducing computational costs compared to conventional ab initio methods. Our electronic DFTB parameters provide reliable predictions for key electronic properties, such as bandgaps and effective masses, closely matching existing experimental data and advanced many body perturbation theory calculations. Furthermore, our approach successfully captures the bandgap trends observed in mixed-halide perovskites, reflecting the variation with halide composition. In addition, we explore the transferability of the newly optimized DFTB parameters to predict the electronic properties of a variety of low-dimensional perovskites and related structures with edge- or face-sharing octahedra.
Article Details
Journal Info
The Journal of Chemical Physics
American Institute of Physics
Authors (14)
Junke Jiang
Univ Rennes, INSA Rennes, CNRS, Institut FOTON–UMR 6082 1 , F-35000 Rennes,
Tammo van der Heide
Institute for Theoretical Physics and Bremen Center for Computational Materials Science, University of Bremen 2 , 28359 Bremen,
Simon Thébaud
Univ Rennes, INSA Rennes, CNRS, Institut FOTON–UMR 6082 1 , F-35000 Rennes,
Carlos Raúl Lien-Medrano
Institute for Theoretical Physics and Bremen Center for Computational Materials Science, University of Bremen 2 , 28359 Bremen,
Arnaud Fihey
Univ Rennes, CNRS, ISCR (Institut des Sciences Chimiques de Rennes)−UMR 6226
Laurent Pedesseau
Univ Rennes, INSA Rennes, CNRS, Institut FOTON–UMR 6082 1 , F-35000 Rennes,
Claudio Quarti
Laboratory for Chemistry of Novel Materials, Materials Research Institute, University of Mons 4 , Place du Parc 20, Mons 7000,
Marios Zacharias
Univ Rennes, INSA Rennes, CNRS, Institut FOTON–UMR 6082 1 , F-35000 Rennes,
George Volonakis
Univ Rennes, ENSCR, INSA Rennes, CNRS, ISCR - UMR 6226
Mikaël Kepenekian
ENSCR, INSA Rennes, CNRS, ISCR (Institut des Sciences Chimiques de Rennes), Univ Rennes, UMR 6226, Rennes F-35000, France
Bálint Aradi
Institute for Theoretical Physics and Bremen Center for Computational Materials Science, University of Bremen 2 , 28359 Bremen,
Michael A. Sentef
Jacky Even
ENSCR, INSA Rennes, CNRS, ISCR (Institut des Sciences Chimiques de Rennes), Univ Rennes, UMR 6226, Rennes F-35000, France
Claudine Katan
Univ Rennes