Controlling Exciton/Exciton Recombination in 2-D Perovskite Using Exciton–Polariton Coupling,The Journal of Physical Chemistry Letters

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Controlling Exciton/Exciton Recombination in 2-D Perovskite Using Exciton–Polariton Coupling
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2024-02-07 , DOI: 10.1021/acs.jpclett.3c03452
Rao Fei _{1,

2} , Matthew P Hautzinger ₁ , Aaron H Rose ₁ , Yifan Dong ₁ , Ivan I Smalyukh _{2,

3,

4,

5} , Matthew C Beard _{1,

5} , Jao van de Lagemaat _{1,

2,

5}

Affiliation

In this paper, we demonstrate that exciton/exciton annihilation in the 2D perovskite (PEA)₂PbI₄ (PEPI)─a major loss mechanism in solar cells and light-emitting diodes, can be controlled through coupling of excitons with cavity polaritons. We study the excited state dynamics using time-resolved transient absorption spectroscopy and show that the system can be tuned through a strong coupling regime by varying the cavity width through the PEPI layer thickness. Remarkably, strong coupling occurs even when the cavity quality factor remains poor, providing easy optical access. We demonstrate that the observed derivative-like transient absorption spectra can be modeled using a time-dependent Rabi splitting that occurs because of transient bleaching of the excitonic states. When PEPI is strongly coupled to the cavity, the exciton/exciton annihilation rate is suppressed by 1 order of magnitude. A model that relies on the partly photonic character of polaritons explains the results as a function of detuning.

中文翻译：

使用激子-极化子耦合控制二维钙钛矿中的激子/激子复合

在本文中，我们证明了二维钙钛矿 (PEA) ₂ PbI ₄ (PEPI) 中的激子/激子湮灭（太阳能电池和发光二极管中的主要损耗机制）可以通过激子与腔极化子的耦合来控制。我们使用时间分辨瞬态吸收光谱研究激发态动力学，并表明可以通过改变 PEPI 层厚度的腔宽度来通过强耦合机制来调整系统。值得注意的是，即使腔体品质因数仍然很差，也会发生强耦合，从而提供轻松的光学接入。我们证明，观察到的类似导数的瞬态吸收光谱可以使用由于激子态的瞬态漂白而发生的时间依赖性拉比分裂来建模。当PEPI与腔强耦合时，激子/激子湮灭率被抑制1个数量级。依赖于极化子部分光子特性的模型将结果解释为失谐的函数。

更新日期：2024-02-07

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