Assessing carrier mobility, dopability, and defect tolerance in the chalcogenide perovskite BaZrS$_3$

Fuente: arXiv
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Main Authors: Yuan, Zhenkun, Dahliah, Diana, Claes, Romain, Pike, Andrew, Fenning, David P., Rignanese, Gian-Marco, Hautier, Geoffroy
Format: Preprint
Published: 2024
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author Yuan, Zhenkun
Dahliah, Diana
Claes, Romain
Pike, Andrew
Fenning, David P.
Rignanese, Gian-Marco
Hautier, Geoffroy
author_facet Yuan, Zhenkun
Dahliah, Diana
Claes, Romain
Pike, Andrew
Fenning, David P.
Rignanese, Gian-Marco
Hautier, Geoffroy
contents The chalcogenide perovskite BaZrS$_3$ has attracted much attention as a promising solar absorber for thin-film photovoltaics. Here, we use first-principles calculations to evaluate its carrier transport and defect properties. We find that BaZrS$_3$ has a phonon-limited electron mobility of 37 cm$^2$/Vs comparable to that in halide perovskites but lower hole mobility of 11 cm$^2$/Vs. The defect computations indicate that BaZrS$_3$ is intrinsically n-type due to shallow sulfur vacancies, but that strong compensation by sulfur vacancies will prevent attempts to make it p-type. We also establish that BaZrS$_3$ shows some degree of defect tolerance, presenting only few low formation energy, deep intrinsic defects. Among the deep defects, sulfur interstitials are the dominant nonradiative recombination centers but exhibit a moderate capture coefficient. Our work highlights the material's intrinsic limitations in carrier mobility and p-type doping and suggests focusing on suppressing the formation of sulfur interstitials to reach longer carrier lifetime.
format Preprint
id arxiv_https___arxiv_org_abs_2405_09793
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle Assessing carrier mobility, dopability, and defect tolerance in the chalcogenide perovskite BaZrS$_3$
Yuan, Zhenkun
Dahliah, Diana
Claes, Romain
Pike, Andrew
Fenning, David P.
Rignanese, Gian-Marco
Hautier, Geoffroy
Materials Science
The chalcogenide perovskite BaZrS$_3$ has attracted much attention as a promising solar absorber for thin-film photovoltaics. Here, we use first-principles calculations to evaluate its carrier transport and defect properties. We find that BaZrS$_3$ has a phonon-limited electron mobility of 37 cm$^2$/Vs comparable to that in halide perovskites but lower hole mobility of 11 cm$^2$/Vs. The defect computations indicate that BaZrS$_3$ is intrinsically n-type due to shallow sulfur vacancies, but that strong compensation by sulfur vacancies will prevent attempts to make it p-type. We also establish that BaZrS$_3$ shows some degree of defect tolerance, presenting only few low formation energy, deep intrinsic defects. Among the deep defects, sulfur interstitials are the dominant nonradiative recombination centers but exhibit a moderate capture coefficient. Our work highlights the material's intrinsic limitations in carrier mobility and p-type doping and suggests focusing on suppressing the formation of sulfur interstitials to reach longer carrier lifetime.
title Assessing carrier mobility, dopability, and defect tolerance in the chalcogenide perovskite BaZrS$_3$
topic Materials Science
url https://arxiv.org/abs/2405.09793