Impact of anharmonicity on the carrier mobility of the Pb-free CsSnBr₃ perovskite

DOI

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.

Identifier
DOI https://doi.org/10.24435/materialscloud:r5-yx
Related Identifier https://archive.materialscloud.org/communities/mcarchive
Related Identifier https://doi.org/10.24435/materialscloud:3e-s3
Metadata Access https://archive.materialscloud.org/oai2d?verb=GetRecord&metadataPrefix=oai_dc&identifier=oai:materialscloud.org:amc23-5wm35
Provenance
Creator Yin, Junwen; Hellman, Olle; Poncé, Samuel
Publisher Materials Cloud
Contributor Yin, Junwen; Hellman, Olle; Poncé, Samuel
Publication Year 2025
Rights info:eu-repo/semantics/openAccess; Creative Commons Attribution 4.0 International; https://creativecommons.org/licenses/by/4.0/legalcode
OpenAccess true
Contact archive(at)materialscloud.org
Representation
Language English
Resource Type info:eu-repo/semantics/other
Format application/gzip; text/markdown
Discipline Materials Science and Engineering