One-Center and Two-Center Self-Trapped Excitons in Zero-Dimensional Hybrid Copper Halides: Tricolor Luminescence with High Quantum Yields
One-Center and Two-Center Self-Trapped Excitons in Zero-Dimensional Hybrid Copper Halides: Tricolor Luminescence with High Quantum Yields
复制标题
零维杂化卤化铜中的一中心和二中心自陷激子：高量子产率的三色发光
DOI：
10.1021/acs.jpclett.2c00002
复制
发表时间：
2022-02-10
影响因子：
5.7
通讯作者：
Fan, Jiyang
中科院分区：
文献类型：
--
作者：
Liu, Xiaoyu;Li, Yuanyuan;Fan, Jiyang
有机-无机杂化卤化铜具有复杂的物理化学性质，其机理尚不清楚。在这里，我们研究了六种新型的低维混合铜卤化物的光动力学，其最大量子产率为98.6%。它们表现出两种不同的温度依赖性和量子跃迁速率的光子发射的起源。结合第一性原理计算的实验结果表明，它们来源于两种自陷激子：单中心a-STE（局域在Cu+单体上）和双中心mSTE（局域在Cu-2（2+）二聚体上）.当获得足够的热能以跨越a-STE和m-STE之间的势垒时，a-STE和m-STE之间存在相变。组成的卤化铜的有机阳离子的柔软度起着关键作用，在确定自陷型的STE。
The organic-inorganic hybrid copper halides exhibit intriguing and complex photophysical properties, and the underlying mechanisms are far from clear. Here, we study the photodynamics of six novel types of low-dimensional hybrid copper halides, which have a maximum quantum yield of 98.6%. They exhibit two origins of photon emission with distinct temperature dependence and quantum transition rates. The experiments in junction with first-principles calculations indicate that they stem from two kinds of self-trapped excitons (STEs): one-center a-STE (localized on Cu+ monomer) and two-center mSTE (localized on Cu-2(2+) dimer). There is phase transition between a-STE and m-STE when enough thermal energy is acquired for crossing the potential barrier between them. The degree of softness of the compositional organic cations of the copper halide plays a key role in determining the self-trapping type of the STEs.