Junwen Yin^1*, Olle Hellman^2*, Samuel Poncé^1,3*

1 European Theoretical Spectroscopy Facility, Institute of Condensed Matter and Nanosciences, Université catholique de Louvain, Chemin des Étoiles 8, B-1348 Louvain-la-Neuve, Belgium.

2 Department of Molecular Chemistry and Materials Science, Weizmann Institute of Science, Rehovot 7610001, Israel.

3 WEL Research Institute, avenue Pasteur 6, 1300 Wavre, Belgique.

* Corresponding authors emails: junwen.yin@uclouvain.be, olle.hellman@liu.se, samuel.ponce@uclouvain.be

DOI10.24435/materialscloud:ha-cb [version v1]

Publication date: May 26, 2025

How to cite this record

Junwen Yin, Olle Hellman, Samuel Poncé, Impact of anharmonicity on the carrier mobility of the Pb-free CsSnBr₃ perovskite, Materials Cloud Archive 2025.84 (2025), https://doi.org/10.24435/materialscloud:ha-cb

Description

Charge carrier mobilities are critical parameters in halide perovskite solar cells, governing their average carrier velocity under an applied electric field and overall efficiency. Recent advances in first-principles calculations of electron-phonon interactions and carrier mobilities have enabled predictive computations for perovskite solar cells. However, the flexible octahedral frameworks and cationic displacements in these materials challenge the harmonic approximation, leading to significant difficulties in accurately calculating transport properties. To address these issues, we combine temperature-dependent effective potentials with the ab initio Boltzmann transport equations to compute carrier mobilities in a representative lead-free perovskite, CsSnBr₃. At room temperature, the electron/hole Hall mobilities in CsSnBr₃ are 106/256 cm²/Vs when neglecting anharmonic effects and 59/145 cm²/Vs when included. This overestimation of the harmonic approximation arises from the neglect of scattering coming from soft modes. We provide a workflow for performing first-principles carrier mobility calculations in anharmonic systems, advancing the predictive modeling of perovskite solar cells.

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Keywords

electron-phonon coupling perovskite mobility anharmonicity ab initio first principles