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Onsite and intersite electronic correlations in the Hubbard model for halide perovskites

Jiyuan Yang1,2, Tianyuan Zhu2,3, Shi Liu2,3*

1 Zhejiang University, Hangzhou, Zhejiang 310058, China

2 Key Laboratory for Quantum Materials of Zhejiang Province, Department of Physics, School of Science, Westlake University, Hangzhou, Zhejiang 310024, China

3 Institute of Natural Sciences, Westlake Institute for Advanced Study, Hangzhou, Zhejiang 310024, China

* Corresponding authors emails: liushi@westlake.edu.cn
DOI10.24435/materialscloud:wt-91 [version v1]

Publication date: Nov 04, 2022

How to cite this record

Jiyuan Yang, Tianyuan Zhu, Shi Liu, Onsite and intersite electronic correlations in the Hubbard model for halide perovskites, Materials Cloud Archive 2022.135 (2022), doi: 10.24435/materialscloud:wt-91.


Halide perovskites (HPs) are widely viewed as promising photovoltaic and light-emitting materials for their suitable band gaps in the visible spectrum. Density functional theory (DFT) calculations employing (semi)local exchange-correlation functionals usually underestimate the band gaps for these systems. Accurate descriptions of the electronic structures of HPs often demand higher-order levels of theory such as the Heyd-Scuseria-Ernzerhof (HSE) hybrid density functional and GW approximations that are much more computationally expensive than standard DFT. Here, we investigate three representative types of HPs, ABX3 halide perovskites, vacancy-ordered double perovskites (VODPs), and bond disproportionated halide perovskites (BDHPs), using DFT+U+V with onsite U and intersite V Hubbard parameters computed self-consistently without a priori assumption. The inclusion of Hubbard corrections improves the band gap prediction accuracy for all three types of HPs to a similar level of advanced methods. Moreover, the self-consistent Hubbard U is a meaningful indicator of the true local charge state of multivalence metal atoms in HPs. The inclusion of the intersite Hubbard V is crucial to properly capture the hybridization between valence electrons on neighboring atoms in BDHPs that have breathing-mode distortions of halide octahedra. In particular, the simultaneous convergence of both Hubbard parameters and crystal geometry enables a band gap prediction accuracy superior to HSE for BDHPs but at a fraction of the cost. Our work highlights the importance of using self-consistent Hubbard parameters when dealing with HPs that often possess intricate competitions between onsite localization and intersite hybridization.

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File name Size Description
12.3 KiB all_structures includes all the structures optimized by PBE (in vasp format)
1.1 MiB An example of DFT+U (QE scripts)
1.1 MiB An example of DFT+U+V (QE scripts)
503 Bytes ReadMe file


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External references

J. Yang, T. Zhu, S. Liu, arXiv:2207.05972 doi:10.48550/arXiv.2207.05972


Halide perovskite DFT+U+V Band gap

Version history:

2022.135 (version v1) [This version] Nov 04, 2022 DOI10.24435/materialscloud:wt-91