Kharintsev Sergey S, Battalova Elina I, Matchenya Ivan A, Nasibulin Albert G, Marunchenko Alexander A, Pushkarev Anatoly P
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.
Adv Sci (Weinh). 2025 Feb;12(5):e2405709. doi: 10.1002/advs.202405709. Epub 2024 Oct 2.
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.
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。
