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无序钙钛矿中的极端电子-光子相互作用

Extreme Electron-Photon Interaction in Disordered Perovskites.

作者信息

Kharintsev Sergey S, Battalova Elina I, Matchenya Ivan A, Nasibulin Albert G, Marunchenko Alexander A, Pushkarev Anatoly P

机构信息

Department of Optics and Nanophotonics, Institute of Physics, Kazan Federal University, Kazan, 420008, Russia.

School of Physics and Engineering, ITMO University, St. Petersburg, 197101, Russia.

出版信息

Adv Sci (Weinh). 2025 Feb;12(5):e2405709. doi: 10.1002/advs.202405709. Epub 2024 Oct 2.

Abstract

The interaction of light with solids can be dramatically enhanced owing to electron-photon momentum matching. This mechanism manifests when light scattering from nanometer-sized clusters including a specific case of self-assembled nanostructures that form a long-range translational order but local disorder (crystal-liquid duality). In this paper, a new strategy based on both cases for the light-matter-interaction enhancement in a direct bandgap semiconductor - lead halide perovskite CsPbBr - by using electric pulse-driven structural disorder, is addressed. The disordered state allows the generation of confined photons, and the formation of an electronic continuum of static/dynamic defect states across the forbidden gap (Urbach bridge). Both mechanisms underlie photon-momentum-enabled electronic Raman scattering (ERS) and single-photon anti-Stokes photoluminescence (PL) under sub-band pump. PL/ERS blinking is discussed to be associated with thermal fluctuations of cross-linked [PbBr] octahedra. Time-delayed synchronization of PL/ERS blinking causes enhanced spontaneous emission at room temperature. These findings indicate the role of photon momentum in enhanced light-matter interactions in disordered and nanostructured solids.

摘要

由于电子 - 光子动量匹配,光与固体之间的相互作用可得到显著增强。当光从纳米尺寸的团簇散射时,这种机制就会显现出来,其中包括一种自组装纳米结构的特定情况,该结构形成长程平移有序但局部无序(晶 - 液二元性)。本文提出了一种基于上述两种情况的新策略,即通过利用电脉冲驱动的结构无序,增强直接带隙半导体——卤化铅钙钛矿CsPbBr中的光 - 物质相互作用。无序状态允许产生受限光子,并在禁带中形成静态/动态缺陷态的电子连续区(乌尔巴赫桥)。这两种机制是子带泵浦下基于光子动量的电子拉曼散射(ERS)和单光子反斯托克斯光致发光(PL)的基础。讨论了PL/ERS闪烁与交联[PbBr]八面体的热涨落有关。PL/ERS闪烁的时间延迟同步导致室温下自发发射增强。这些发现表明了光子动量在无序和纳米结构固体中增强光 - 物质相互作用方面的作用。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ff7f/11792048/f31f56996bce/ADVS-12-2405709-g001.jpg

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