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卤化铅钙钛矿中电子和空穴的朗德因子:对带隙的普遍依赖关系。

The Landé factors of electrons and holes in lead halide perovskites: universal dependence on the band gap.

作者信息

Kirstein E, Yakovlev D R, Glazov M M, Zhukov E A, Kudlacik D, Kalitukha I V, Sapega V F, Dimitriev G S, Semina M A, Nestoklon M O, Ivchenko E L, Kopteva N E, Dirin D N, Nazarenko O, Kovalenko M V, Baumann A, Höcker J, Dyakonov V, Bayer M

机构信息

Experimentelle Physik 2, Technische Universität Dortmund, 44227, Dortmund, Germany.

Ioffe Institute, Russian Academy of Sciences, 194021, St. Petersburg, Russia.

出版信息

Nat Commun. 2022 Jun 2;13(1):3062. doi: 10.1038/s41467-022-30701-0.

Abstract

The Landé or g-factors of charge carriers are decisive for the spin-dependent phenomena in solids and provide also information about the underlying electronic band structure. We present a comprehensive set of experimental data for values and anisotropies of the electron and hole Landé factors in hybrid organic-inorganic (MAPbI, MAPb(BrCl), MAPb(BrCl), FAPbBr, FACsPbIBr, MA=methylammonium and FA=formamidinium) and all-inorganic (CsPbBr) lead halide perovskites, determined by pump-probe Kerr rotation and spin-flip Raman scattering in magnetic fields up to 10 T at cryogenic temperatures. Further, we use first-principles density functional theory (DFT) calculations in combination with tight-binding and k ⋅ p approaches to calculate microscopically the Landé factors. The results demonstrate their universal dependence on the band gap energy across the different perovskite material classes, which can be summarized in a universal semi-phenomenological expression, in good agreement with experiment.

摘要

电荷载流子的朗德g因子对于固体中的自旋相关现象起着决定性作用,同时也提供了有关潜在电子能带结构的信息。我们展示了一组全面的实验数据,这些数据是关于混合有机-无机(MAPbI、MAPb(BrCl)、MAPb(BrCl)、FAPbBr、FACsPbIBr,MA = 甲基铵,FA = 甲脒)和全无机(CsPbBr)卤化铅钙钛矿中电子和空穴朗德因子的值及各向异性,这些数据是在低温下通过泵浦-探测克尔旋转和在高达10 T的磁场中的自旋翻转拉曼散射测定的。此外,我们结合紧束缚和k·p方法使用第一性原理密度泛函理论(DFT)计算来微观计算朗德因子。结果表明,它们普遍依赖于不同钙钛矿材料类别的带隙能量,这可以用一个通用的半唯象表达式来概括,与实验结果吻合良好。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/aa8d/9163162/90c21ca20bfb/41467_2022_30701_Fig1_HTML.jpg

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