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钙钛矿纳米晶的单光子发射与尺寸的相关性。

Correlation between Single-Photon Emission and Size of Cesium Lead Bromide Perovskite Nanocrystals.

机构信息

Department of Applied Chemistry for Environment, Kwansei Gakuin University, 1 Gakuen Uegahara, Sanda, Hyogo 669-1330, Japan.

出版信息

J Phys Chem Lett. 2023 Mar 9;14(9):2441-2447. doi: 10.1021/acs.jpclett.3c00059. Epub 2023 Mar 2.

Abstract

Emission photon statistics of semiconductor nanocrystal quantum dots (QDs), including lead halide perovskite nanocrystals (PNCs), are important fundamental and practical optical properties. Single QDs exhibit high-probability single-photon emission owing to the efficient Auger recombination between generated excitons. Because the recombination rate depends on QD size, single-photon emission probability should be size-dependent. Previous studies have researched QDs smaller than their exciton Bohr diameters (twice the Bohr radius of excitons). Here, we investigated the relationship between the single-photon emission behavior and size of CsPbBr PNCs to elucidate their size threshold. Simultaneous single-nanocrystal spectroscopy and atomic force microscopy observations on single PNCs with approximately 5-25 nm edge length showed that those smaller than approximately 10 nm, which had size-dependent photoluminescence (PL) spectral shifts, exhibited high-probability single-photon emissions, which decreased linearly with PNC volume. Novel single-photon emission, size, and PL peak correlations of PNCs are important for understanding the relationship between single-photon emission and quantum confinement.

摘要

半导体纳米晶量子点(QDs)的发射光子统计特性,包括卤化铅钙钛矿纳米晶(PNCs),是重要的基本和实际光学性质。由于激子产生的高效俄歇复合,单个 QD 表现出高概率的单光子发射。由于复合速率取决于 QD 的尺寸,因此单光子发射概率应该是尺寸依赖性的。以前的研究已经研究了小于激子玻尔直径(激子玻尔半径的两倍)的 QD。在这里,我们研究了单光子发射行为与 CsPbBr PNC 尺寸之间的关系,以阐明其尺寸阈值。通过对具有约 5-25nm 边缘长度的单个 PNC 进行同时单纳米晶体光谱学和原子力显微镜观测,我们发现那些小于约 10nm 的 PNC 具有尺寸依赖性的光致发光(PL)光谱位移,表现出高概率的单光子发射,其随 PNC 体积呈线性下降。PNC 的单光子发射、尺寸和 PL 峰的新关联对于理解单光子发射与量子限制之间的关系很重要。

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