Enhanced photoluminescence quantum yield in metal halide perovskites via trace Ag doping

IF 7.4 2区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Science China Materials Pub Date : 2025-07-07 DOI:10.1007/s40843-025-3458-1

Machao Wang (, ), Yangmin Tang (, ), Guiqiang Pu (, ), Chengbin Kang (, ), Zhiqiang Wang (, ), Lijia Liu (, ), Jing Li (, ), Zhenzhen Zhou (, ), Wei Chen (, ), Dong Wang (, ), Jiacheng Wang (, )

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引用次数: 0

Abstract

Self-trapped excitons are prevalent in metal halide perovskites (MHPs) characterized by soft lattices and strong exciton-phonon coupling, emitting photons with broadband emission and large Stokes shifts, rendering them particularly well-suited for applications in light-emitting diodes. But their photoluminescence quantum yields (PLQY) are limited by both high exciton binding energy and halogen-vacancy-associated non-radiative recombination. Here, we show that PLQY could be enhanced by a factor of 5.6 from 16% to 89% through doping trace Ag into Cs₂NaBiCl₆ double perovskites, superior to those of previous Cs₂NaBiCl₆-based emitters. Experimental and theoretical studies reveal that trace Ag-initiated covalent interactions could reduce the exciton binding energy by 0.12 eV due to local symmetry breaking, thus improving the photoexcitation process. Also, this covalent interaction could passivate Cl vacancy defects, suppressing non-radiative recombination. Therefore, Cs₂NaBiCl₆: 0.7% Ag⁺ could accumulate active self-trapped excitons to obtain high PLQY. Assembly of near-infrared light-emitting diodes using Cs₂NaBiCl₆: 0.7% Ag⁺ illustrates their valuable applications in nondestructive spectral analysis and night vision illumination. This work shows an effective strategy of improving photoemission of MHPs with high PLQY for advanced optoelectronic applications.

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微量银掺杂提高金属卤化物钙钛矿的光致发光量子产率

自捕获激子普遍存在于金属卤化物钙钛矿（MHPs）中，其特征是软晶格和强激子-声子耦合，发射具有宽带发射和大斯托克斯位移的光子，使它们特别适合于发光二极管的应用。但它们的光致发光量子产率（PLQY）受到高激子结合能和卤素空位相关的非辐射复合的限制。在这里，我们发现通过在Cs2NaBiCl6双钙钛矿中掺杂痕量Ag可以将PLQY从16%提高到89%，提高了5.6倍，优于以前基于Cs2NaBiCl6的发射体。实验和理论研究表明，微量银引发的共价相互作用由于局部对称性破缺，使激子结合能降低0.12 eV，从而改善了光激发过程。此外，这种共价相互作用可以钝化Cl空位缺陷，抑制非辐射复合。因此，Cs2NaBiCl6: 0.7% Ag+可以积累活跃的自捕获激子，从而获得高PLQY。用Cs2NaBiCl6: 0.7% Ag+组装近红外发光二极管，说明了其在无损光谱分析和夜视照明方面的宝贵应用。这项工作为先进光电应用提供了一种有效的策略，可以改善具有高PLQY的MHPs的光电发射。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Science China Materials Materials Science-General Materials Science

CiteScore

11.40

自引率

7.40%

发文量

949

期刊介绍： Science China Materials (SCM) is a globally peer-reviewed journal that covers all facets of materials science. It is supervised by the Chinese Academy of Sciences and co-sponsored by the Chinese Academy of Sciences and the National Natural Science Foundation of China. The journal is jointly published monthly in both printed and electronic forms by Science China Press and Springer. The aim of SCM is to encourage communication of high-quality, innovative research results at the cutting-edge interface of materials science with chemistry, physics, biology, and engineering. It focuses on breakthroughs from around the world and aims to become a world-leading academic journal for materials science.