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常规三维溴化铅钙钛矿纳米晶体在高压下的自陷激子发射和压致变色

Self-trapped exciton emission and piezochromism in conventional 3D lead bromide perovskite nanocrystals under high pressure.

作者信息

Shi Yue, Zhao Wenya, Ma Zhiwei, Xiao Guanjun, Zou Bo

机构信息

State Key Laboratory of Superhard Materials, College of Physics, Jilin University Changchun 130012 China

出版信息

Chem Sci. 2021 Oct 21;12(44):14711-14717. doi: 10.1039/d1sc04987a. eCollection 2021 Nov 17.

Abstract

Developing single-component materials with bright-white emission is required for energy-saving applications. Self-trapped exciton (STE) emission is regarded as a robust way to generate intrinsic white light in halide perovskites. However, STE emission usually occurs in low-dimensional perovskites whereby a lower level of structural connectivity reduces the conductivity. Enabling conventional three-dimensional (3D) perovskites to produce STEs to elicit competitive white emission is challenging. Here, we first achieved STEs-related emission of white light with outstanding chromaticity coordinates of (0.330, 0.325) in typical 3D perovskites, Mn-doped CsPbBr nanocrystals (NCs), through pressure processing. Remarkable piezochromism from red to blue was also realized in compressed Mn-doped CsPbBr NCs. Doping engineering by size-mismatched Mn dopants could give rise to the formation of localized carriers. Hence, high pressure could further induce octahedra distortion to accommodate the STEs, which has never occurred in pure 3D perovskites. Our study not only offers deep insights into the photophysical nature of perovskites, it also provides a promising strategy towards high-quality, stable white-light emission.

摘要

节能应用需要开发具有亮白色发射的单组分材料。自陷激子(STE)发射被认为是在卤化物钙钛矿中产生本征白光的一种有效方式。然而,STE发射通常发生在低维钙钛矿中,较低的结构连通性会降低其导电性。使传统的三维(3D)钙钛矿产生STE以引发具有竞争力的白色发射具有挑战性。在此,我们首次通过压力处理在典型的3D钙钛矿、锰掺杂的CsPbBr纳米晶体(NCs)中实现了与STE相关的白光发射,其色度坐标出色,为(0.330, 0.325)。在压缩的锰掺杂CsPbBr NCs中还实现了从红色到蓝色的显著压致变色。由尺寸不匹配的锰掺杂剂进行的掺杂工程可导致局域载流子的形成。因此,高压可进一步诱导八面体畸变以容纳STE,这在纯3D钙钛矿中从未发生过。我们的研究不仅深入洞察了钙钛矿的光物理性质,还为高质量、稳定的白光发射提供了一种有前景的策略。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e940/8597834/40dfeaa74a85/d1sc04987a-f1.jpg

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