Enhanced Charge Transport in A-site Ordered Perovskite Derivatives A2A'Bi2I9 (A = Cs; A'= Ag, Cu): A First-Principles Study

Fuente: arXiv
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Autori principali: Li, Shuhan, Song, Siyu, Lv, Peng, Wang, Shihao, Hong, Jiawang, Tang, Gang
Natura: Preprint
Pubblicazione: 2025
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author Li, Shuhan
Song, Siyu
Lv, Peng
Wang, Shihao
Hong, Jiawang
Tang, Gang
author_facet Li, Shuhan
Song, Siyu
Lv, Peng
Wang, Shihao
Hong, Jiawang
Tang, Gang
contents Recent experiments have synthesized Cs2AgBi2I9 by partially substituting Cs+ with Ag+ at the A-site of Cs3Bi2I9, resulting in enhanced charge transport properties compared to Cs3Bi2I9. However, the atomic-scale mechanisms behind this enhancement remain unclear. In this work, we investigate the carrier transport mechanisms in Cs2A'Bi2I9 (A' = Ag, Cu) using first-principles calculations and Boltzmann transport calculations. Our results reveal that A-site ordered Cs2A'Bi2I9 exhibits carrier mobilities that are 3-4 times higher than those of Cs3Bi2I9 within the 100-500 K temperature range. We identify polar phonon scattering as the dominant mechanism limiting mobility. Furthermore, the enhanced out-of-plane carrier mobility in Cs2A'Bi2I9, particularly between 100 and 200K, leads to reduced mobility anisotropy. These improvements are mainly due to the shorter A'-I bond lengths and increased Ag+/Cu+ s-I p orbital coupling. Notably, substitution with Cu+ results in a further reduction in the band gap and enhanced hole mobility compared to Ag+ substitution in Cs3Bi2I9. Further analysis reveals that the significant increase in carrier mobility in Cs2A'Bi2I9 can be largely explained by the smaller carrier effective masses (m*) and weaker Fröhlich coupling strengths (α), resulting in a lower polar mass α(m*/me), compared to Cs3Bi2I9. Our study provides valuable insights into the transport properties of Bi-based perovskite derivatives, paving the way for their future applications in optoelectronic devices.
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id arxiv_https___arxiv_org_abs_2503_02478
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Enhanced Charge Transport in A-site Ordered Perovskite Derivatives A2A'Bi2I9 (A = Cs; A'= Ag, Cu): A First-Principles Study
Li, Shuhan
Song, Siyu
Lv, Peng
Wang, Shihao
Hong, Jiawang
Tang, Gang
Materials Science
Recent experiments have synthesized Cs2AgBi2I9 by partially substituting Cs+ with Ag+ at the A-site of Cs3Bi2I9, resulting in enhanced charge transport properties compared to Cs3Bi2I9. However, the atomic-scale mechanisms behind this enhancement remain unclear. In this work, we investigate the carrier transport mechanisms in Cs2A'Bi2I9 (A' = Ag, Cu) using first-principles calculations and Boltzmann transport calculations. Our results reveal that A-site ordered Cs2A'Bi2I9 exhibits carrier mobilities that are 3-4 times higher than those of Cs3Bi2I9 within the 100-500 K temperature range. We identify polar phonon scattering as the dominant mechanism limiting mobility. Furthermore, the enhanced out-of-plane carrier mobility in Cs2A'Bi2I9, particularly between 100 and 200K, leads to reduced mobility anisotropy. These improvements are mainly due to the shorter A'-I bond lengths and increased Ag+/Cu+ s-I p orbital coupling. Notably, substitution with Cu+ results in a further reduction in the band gap and enhanced hole mobility compared to Ag+ substitution in Cs3Bi2I9. Further analysis reveals that the significant increase in carrier mobility in Cs2A'Bi2I9 can be largely explained by the smaller carrier effective masses (m*) and weaker Fröhlich coupling strengths (α), resulting in a lower polar mass α(m*/me), compared to Cs3Bi2I9. Our study provides valuable insights into the transport properties of Bi-based perovskite derivatives, paving the way for their future applications in optoelectronic devices.
title Enhanced Charge Transport in A-site Ordered Perovskite Derivatives A2A'Bi2I9 (A = Cs; A'= Ag, Cu): A First-Principles Study
topic Materials Science
url https://arxiv.org/abs/2503.02478