Converting Self-Trapped Exciton from Dark to Bright State via Excessive Eu Incorporation in CsEuCl 3 Nanocrystals

激子 材料科学 光电子学 自发辐射 二极管 光致发光 卤化物 钙钛矿(结构) 量子点 量子产额 纳米晶 飞秒 吸收(声学) 发射光谱 发射强度 超快激光光谱学 发光 格子(音乐) 光发射 发光二极管 基态 产量(工程) 吸收光谱法 化学物理 辐射传输 分子物理学
作者
Wanxin Zhuang,M. Li,Qiuyan Cen,You-Liang Zhu,Dan Yao,Hao Zhang
出处
期刊:Journal of Physical Chemistry Letters [American Chemical Society]
卷期号:17 (14): 4089-4099 被引量:1
标识
DOI:10.1021/acs.jpclett.6c00722
摘要

CsEuCl 3 nanocrystals (NCs) are novel lead-free rare-earth perovskite NCs with low toxicity and intrinsic optical activity, exhibiting potential as promising alternatives to lead halide perovskites. However, the limited understanding of their dual-photoluminescence (PL) emission mechanism impedes further material optimization and device integration of CsEuCl 3 NCs. In this work, the origin of the dual PL emission peaks in CsEuCl 3 NCs is elucidated through comprehensive spectroscopic analyses, including femtosecond transient absorption and temperature-dependent PL spectroscopy. The narrow emission at 435 nm is identified as the band-edge free-exciton recombination, while the broad emission centered at 559 nm arises from extrinsic self-trapped exciton (STE) emission. The excessive Eu suppresses lattice vibrations and facilitates the conversion of the dark STE state into a radiative bright state, thereby enhancing the PL quantum yield (PLQY) to 34.1%, which is record-high for CsEuCl 3 NCs. By systematic tuning of the Eu content, the intensity ratio between dual emission bands is regulated. On the basis of the tunable emission, white-light-emitting diodes with correlated color temperatures of 8788 to 4371 K and high operation stability are successfully fabricated. This work unveils the fundamental mechanism governing dual emission behavior in CsEuCl 3 NCs, establishes an effective strategy for PL modulation, and highlights their potential as robust, lead-free materials for next-generation solid-state lighting applications.
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