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二维（PEA）PbI钙钛矿中的 Rashba 型能带分裂效应及其对激子 - 声子耦合的影响。

Rashba-Type Band Splitting Effect in 2D (PEA)PbI Perovskites and Its Impact on Exciton-Phonon Coupling.

作者信息

Ghosh Supriya, Pradhan Bapi, Bandyopadhyay Arkamita, Skvortsova Irina, Zhang Yiyue, Sternemann Christian, Paulus Michael, Bals Sara, Hofkens Johan, Karki Khadga J, Materny Arnulf

机构信息

School of Science, Constructor University, Campus Ring 1, 28759 Bremen, Germany.

Department of Chemistry and Biochemistry, The Ohio State University, 100 West 18th Avenue, Columbus, Ohio 43210, United States.

出版信息

J Phys Chem Lett. 2024 Aug 8;15(31):7970-7978. doi: 10.1021/acs.jpclett.4c01957. Epub 2024 Jul 30.

DOI:10.1021/acs.jpclett.4c01957
PMID:39077842
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11318034/
Abstract

Despite a few recent reports on Rashba effects in two-dimensional (2D) Ruddlesden-Popper (RP) hybrid perovskites, the precise role of organic spacer cations in influencing Rashba band splitting remains unclear. Here, using a combination of temperature-dependent two-photon photoluminescence (2PPL) and time-resolved photoluminescence spectroscopy, alongside density functional theory (DFT) calculations, we contribute to significant insights into the Rashba band splitting found for 2D RP hybrid perovskites. The results demonstrate that the polarity of the organic spacer cation is crucial in inducing structural distortions that lead to Rashba-type band splitting. Our investigations show that the intricate details of the Rashba band splitting occur for organic cations with low polarity but not for more polar ones. Furthermore, we have observed stronger exciton-phonon interactions due to the Rashba-type band splitting effect. These findings clarify the importance of selecting appropriate organic spacer cations to manipulate the electronic properties of 2D perovskites.

摘要

尽管最近有一些关于二维（2D）Ruddlesden-Popper（RP）杂化钙钛矿中 Rashba 效应的报道，但有机间隔阳离子在影响 Rashba 能带分裂方面的确切作用仍不清楚。在这里，我们结合温度依赖的双光子光致发光（2PPL）和时间分辨光致发光光谱，以及密度泛函理论（DFT）计算，对二维 RP 杂化钙钛矿中发现的 Rashba 能带分裂有了重要的见解。结果表明，有机间隔阳离子的极性对于诱导导致 Rashba 型能带分裂的结构畸变至关重要。我们的研究表明，Rashba 能带分裂的复杂细节发生在低极性有机阳离子中，而不是极性更强的阳离子中。此外，由于 Rashba 型能带分裂效应，我们观察到了更强的激子 - 声子相互作用。这些发现阐明了选择合适的有机间隔阳离子来操纵二维钙钛矿电子性质的重要性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1e63/11318034/aefd624b2300/jz4c01957_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1e63/11318034/a0bf26886de0/jz4c01957_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1e63/11318034/7f8619145826/jz4c01957_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1e63/11318034/2a33992d45b8/jz4c01957_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1e63/11318034/870f01df3896/jz4c01957_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1e63/11318034/500518ffa4cd/jz4c01957_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1e63/11318034/aefd624b2300/jz4c01957_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1e63/11318034/a0bf26886de0/jz4c01957_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1e63/11318034/7f8619145826/jz4c01957_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1e63/11318034/2a33992d45b8/jz4c01957_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1e63/11318034/870f01df3896/jz4c01957_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1e63/11318034/500518ffa4cd/jz4c01957_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1e63/11318034/aefd624b2300/jz4c01957_0006.jpg

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本文引用的文献

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Lattice Dynamics and Electron-Phonon Coupling in Double Perovskite CsNaFeCl.双钙钛矿CsNaFeCl中的晶格动力学与电子-声子耦合
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Slower Auger Recombination in 12-Faceted Dodecahedron CsPbBr Nanocrystals.
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Rashba splitting in organic-inorganic lead-halide perovskites revealed through two-photon absorption spectroscopy.通过双光子吸收光谱揭示有机-无机铅卤化物钙钛矿中的 Rashba 分裂
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