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Exploring Orbit-Orbit Interaction in Relationship to Photoluminescence Quantum Efficiency in Perovskite Quantum Dots through Rashba Effect.
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2019-12-11 , DOI: 10.1021/acs.jpclett.9b02936
Hengxing Xu 1 , Prem Prabhakaran 2 , Sinil Choi 2 , Miaosheng Wang 1 , Kwang-Sup Lee 2 , Bin Hu 1
Affiliation  

This study demonstrates the influence of the orbit-orbit interaction on the photoluminescence quantum efficiency (PLQE) of metal halide perovskite quantum dots (QDs) through the Rashba effect. The orbit-orbit interaction between excitons was characterized by using the minimal excitation intensity required to generate a photoluminescence difference (ΔPL) between linearly and circularly polarized photoexcitations. It was observed that changing the surface functionalization from PFOA-OA to PFSH-OAm and OA can largely increase the minimal excitation intensity for generating ΔPL. This indicates that the orbit-orbit interaction is essentially decreased in CsPbBr1I2 QDs with surface functionalization. Simultaneously, the PLQE is increased from 39% to 59 and 72% in CsPbBr1I2 QDs upon surface functionalization. Furthermore, the PL lifetime is decreased with increasing the PLQE in CsPbBr1I2 QDs upon surface functionalization. This phenomenon implies that decreasing the orbit-orbit interaction can essentially weaken the Rashba effect and consequently reduce the disallowed transitions, leading to an enhancement in the PLQE in perovskite QDs.

中文翻译:

通过Rashba效应探索钙钛矿量子点中与光致发光量子效率相关的轨道-轨道相互作用。

这项研究通过Rashba效应证明了轨道-轨道相互作用对金属卤化物钙钛矿量子点(QDs)的光致发光量子效率(PLQE)的影响。激子之间的轨道-轨道相互作用通过使用产生线性和圆偏振光激发之间的光致发光差异(ΔPL)所需的最小激发强度来表征。观察到,将表面官能化从PFOA-OA更改为PFSH-OAm和OA可以大大增加产生ΔPL的最小激发强度。这表明在具有表面功能化的CsPbBr1I2 QD中,轨道与轨道之间的相互作用实质上得到了降低。同时,表面功能化后,CsPbBr1I2 QD中的PLQE从39%增加到59和72%。此外,表面功能化后,PL寿命随着CsPbBr1I2 QD中PLQE的增加而降低。这种现象表明,减少轨道与轨道的相互作用会实质上削弱拉什巴效应,从而减少不允许的跃迁,从而导致钙钛矿量子点的PLQE增强。
更新日期:2019-12-13
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