强约束CsPbBr3纳米晶体自旋弛豫动力学的超快光谱分析

IF 4.6 2区化学 Q1 SPECTROSCOPY

Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy Pub Date : 2025-06-03 DOI:10.1016/j.saa.2025.126534

Zixiang Zhou , Rongxin Zhang , Lei Wang, Xin Zhang, Meihua Chen, Zixi Yin, Ying Liang, Guijie Liang

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引用次数: 0

摘要

由于卤化铅钙钛矿（LHPs）中自旋极化态的光学取向很容易，因此在自旋电子学或量子信息科学的应用中，人们一直致力于有效的自旋探测和操纵。在研究激子自旋动力学的常用表征方法中，圆极化瞬态吸收光谱（CPTA）是一种重要的表征方法。本文合成了3个小尺寸CsPbBr3纳米晶体（NCs）（3.2 ~ 4.3 nm），并利用CPTA光谱分析了它们的自旋弛豫动力学。结果表明，对于具有强量子约束的CsPbBr3 NCs，特别是对于3.2 nm的CsPbBr3，在较大波长下由第二次光诱导吸收（PA2）动力学得到的自旋弛豫时间远长于第一次激子漂白（XB）和第一次光诱导吸收（PA1）得到的自旋弛豫时间。换句话说，PA2动力学可以更准确地反映强约束nc中的自旋弛豫过程。这一现象可归因于PA2动力学中带边激子之间的库仑相互作用占主导地位，而XB和PA1的其他两个动力学对热激子弛豫更为敏感。考虑到由于合成困难而导致小尺寸非均匀性普遍存在的问题，本研究可以为利用CPTA光谱探索强约束LHPs NCs中的自旋弛豫动力学提供进一步的见解，并有利于自旋电子学或量子信息科学的相关应用。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

Ultrafast spectral analysis on the spin relaxation dynamics in strongly confined CsPbBr3 nanocrystals

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Ultrafast spectral analysis on the spin relaxation dynamics in strongly confined CsPbBr3 nanocrystals

Owing to the facile optical orientation of spin-polarized states in lead halide perovskites (LHPs), extensive efforts have been devoted to their efficient spin detection and manipulation for applications of spintronics or quantum information science. Among usual characterization methods for exploring the exciton spin dynamics, the circularly polarized transient absorption (CPTA) spectroscopy is an important one. Herein, three small-sized CsPbBr₃ nanocrystals (NCs) (3.2–4.3 nm) are synthesized and their spin relaxation dynamics are analyzed by employing CPTA spectroscopy. The results reveal that for CsPbBr₃ NCs with strong quantum confinement, expecially for the 3.2 nm CsPbBr₃, the spin relaxation time derived from the second photo-induced absorption (PA2) kinetics at larger wavelength is much longer than those from the first exciton bleach (XB) and the first photo-induced absorption (PA1). In other words, the PA2 kinetics can reflect more accurate spin relaxation process in strongly confined NCs. This phenomenen can be attributed to the dominant Coulomb interaction between the band edge excitons for PA2 kinetics, while the other two kinetics of XB and PA1 are more sensitive to hot exciton relaxation. Considering the common issues that inhomogeneity generally exists in small-sized NCs due to difficult synthesis, this study could provide further insight for exploring the spin relaxation dynamics by CPTA spectroscopy in strongly confined LHPs NCs and benefit related applications in spintronics or quantum information science.

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来源期刊

Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy 物理-光谱学

CiteScore

8.40

自引率

11.40%

发文量

1364

审稿时长

40 days

期刊介绍： Spectrochimica Acta, Part A: Molecular and Biomolecular Spectroscopy (SAA) is an interdisciplinary journal which spans from basic to applied aspects of optical spectroscopy in chemistry, medicine, biology, and materials science. The journal publishes original scientific papers that feature high-quality spectroscopic data and analysis. From the broad range of optical spectroscopies, the emphasis is on electronic, vibrational or rotational spectra of molecules, rather than on spectroscopy based on magnetic moments. Criteria for publication in SAA are novelty, uniqueness, and outstanding quality. Routine applications of spectroscopic techniques and computational methods are not appropriate. Topics of particular interest of Spectrochimica Acta Part A include, but are not limited to: Spectroscopy and dynamics of bioanalytical, biomedical, environmental, and atmospheric sciences, Novel experimental techniques or instrumentation for molecular spectroscopy, Novel theoretical and computational methods, Novel applications in photochemistry and photobiology, Novel interpretational approaches as well as advances in data analysis based on electronic or vibrational spectroscopy.