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压力对强量子限域CsPbBr量子点和纳米片激子吸收与发射的影响

Effects of Pressure on Exciton Absorption and Emission in Strongly Quantum-Confined CsPbBr Quantum Dots and Nanoplatelets.

作者信息

Wang Chih-Wei, Oyeka Ebube E, Altman Alison B, Son Dong Hee

机构信息

Department of Chemistry, Texas A&M University, College Station, Texas 77843, United States.

Department of Physics and Astronomy, Texas A&M University, College Station, Texas 77843, United States.

出版信息

J Phys Chem C Nanomater Interfaces. 2024 Jan 31;128(5):2062-2069. doi: 10.1021/acs.jpcc.3c08029. eCollection 2024 Feb 8.

Abstract

Soft lattices of metal halide perovskite (MHP) nanocrystals (NCs) are considered responsible for many of their optical properties associated with excitons, which are often distinct from other semiconductor NCs. Earlier studies of MHP NCs upon compression revealed how structural changes and the resulting changes in the optical properties such as the bandgap can be induced at relatively low pressures. However, the pressure response of the exciton transition itself in MHP NCs remains relatively poorly understood due to limitations inherent to studying weakly or nonconfined NCs in which exciton absorption peaks are not well-separated from the continuum interband transition. Here, we investigated the pressure response of the absorbing and emitting transitions of excitons using strongly quantum-confined CsPbBr quantum dots (QDs) and nanoplatelets (NPLs), which both exhibit well-defined exciton absorption peaks. Notably, the reversible vanishing and recovery of the exciton absorption accompanied by reversible quenching and recovery of the emission were observed in both QDs and NPLs, resulting from the reversible pressure modulation of the exciton oscillator strength. Furthermore, CsPbBr NPLs exhibited irreversible pressure-induced creation of trap states at low pressures (∼0.1 GPa) responsible for trapped exciton emission that developed on the time scale of ∼10 min, while the reversible pressure response of the absorbing exciton transition was maintained. These findings shed light on the diverse effects the application of force has on the absorbing and emitting exciton transitions in MHP NCs, which are important for their application as excitonic light emitters in high-pressure environments.

摘要

金属卤化物钙钛矿(MHP)纳米晶体(NCs)的软晶格被认为是其许多与激子相关的光学性质的原因,这些性质通常与其他半导体NCs不同。早期对MHP NCs压缩的研究揭示了在相对较低压力下如何诱导结构变化以及由此产生的光学性质变化,如带隙变化。然而,由于研究弱约束或无约束NCs存在固有局限性,其中激子吸收峰与连续带间跃迁没有很好地分离,MHP NCs中激子跃迁本身的压力响应仍相对了解不足。在这里,我们使用强量子约束的CsPbBr量子点(QDs)和纳米片(NPLs)研究了激子吸收和发射跃迁的压力响应,它们都表现出明确的激子吸收峰。值得注意的是,在QDs和NPLs中都观察到激子吸收的可逆消失和恢复,伴随着发射的可逆猝灭和恢复,这是由激子振子强度的可逆压力调制引起的。此外,CsPbBr NPLs在低压(约0.1 GPa)下表现出不可逆的压力诱导陷阱态的产生,这些陷阱态导致在约10分钟的时间尺度上出现捕获激子发射,同时吸收激子跃迁的可逆压力响应得以维持。这些发现揭示了施加力对MHP NCs中吸收和发射激子跃迁的多种影响,这对于它们在高压环境中作为激子发光体的应用很重要。

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