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FAPbBr钙钛矿晶体中的相干载流子自旋动力学

Coherent Carrier Spin Dynamics in FAPbBr Perovskite Crystals.

作者信息

Kirstein Erik, Zhukov Evgeny A, Yakovlev Dmitri R, Kopteva Nataliia E, Yalcin Eyüp, Akimov Ilya A, Hordiichuk Oleh, Dirin Dmitry N, Kovalenko Maksym V, Bayer Manfred

机构信息

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

Department of Chemistry and Applied Biosciences, Laboratory of Inorganic Chemistry, ETH Zürich, CH-8093 Zürich,Switzerland.

出版信息

J Phys Chem Lett. 2024 Mar 14;15(10):2893-2903. doi: 10.1021/acs.jpclett.4c00098. Epub 2024 Mar 6.

Abstract

Coherent spin dynamics of electrons and holes are studied in hybrid organic-inorganic lead halide perovskite FAPbBr bulk single crystals using the time-resolved Kerr ellipticity technique at cryogenic temperatures. The Larmor spin precession of the carrier spins in a magnetic field is monitored to measure the Landé -factors of electrons (+2.44) and holes (+0.41). These -factors are highly isotropic. The measured spin dephasing times amount to a few nanoseconds, and the longitudinal hole spin relaxation time is 470 ns. The important role of the strong hyperfine interaction between carrier spins and nuclear spins is demonstrated via dynamic nuclear polarization. At low temperatures, electron and hole spin relaxation predominantly occurs via the hyperfine interaction, whose importance significantly decreases at temperatures above 12 K. We overview the spin dynamics in various lead halide perovskite crystals and polycrystalline films and conclude on their common features provided by charge carrier localization at cryogenic temperatures.

摘要

在低温下,使用时间分辨克尔椭圆率技术研究了有机-无机杂化卤化铅钙钛矿FAPbBr块状单晶中电子和空穴的相干自旋动力学。监测磁场中载流子自旋的拉莫尔自旋进动,以测量电子(+2.44)和空穴(+0.41)的朗德因子。这些因子具有高度各向同性。测得的自旋退相时间为几纳秒,纵向空穴自旋弛豫时间为470纳秒。通过动态核极化证明了载流子自旋与核自旋之间强超精细相互作用的重要作用。在低温下,电子和空穴自旋弛豫主要通过超精细相互作用发生,在高于12 K的温度下,其重要性显著降低。我们概述了各种卤化铅钙钛矿晶体和多晶薄膜中的自旋动力学,并总结了低温下电荷载流子局域化所提供的共同特征。

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