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Correlated Self-Trapped Excitons and Free Excitons with Intermediate Exciton–Phonon Coupling in 2D Mixed-Halide Perovskites
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2023-11-01 , DOI: 10.1021/acs.jpclett.3c02346 Cheng Yang 1 , Qi Wei 2 , Yiyang Gong 1 , Mingzhu Long 1 , Guofu Zhou 1 , Guichuan Xing 2 , Bo Wu 1
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2023-11-01 , DOI: 10.1021/acs.jpclett.3c02346 Cheng Yang 1 , Qi Wei 2 , Yiyang Gong 1 , Mingzhu Long 1 , Guofu Zhou 1 , Guichuan Xing 2 , Bo Wu 1
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Low-dimensional lead halides have attracted increasing attention due to their potential application as single-component white-light emitters. These materials exhibit a complex emission spectral structure, ranging from free exciton narrowband emissions to self-trapped exciton broadband emissions. However, there is still no consensus for the underlying physical mechanism, especially in the spectrum with both narrowband and broadband emissions. Here we aim to elucidate the correlation between the emission spectrum and the exciton–phonon coupling in the mixed halide perovskite BA2Pb(BrxCl1–x)4. Our findings reveal that the interplay between exciton localization and delocalization results in an intermediate exciton–phonon coupling, leading to line shapes beyond the Huang–Rhys model for the self-trapped exciton. By incorporating the exciton motional effect, we establish a unified photophysical model describing the emission spectrum from the self-trapped exciton type to the free exciton type. These results provide essential insights into the mechanisms governing exciton–phonon interactions and offer ways to control white-light emission in two-dimensional perovskites.
中文翻译：
二维混合卤化物钙钛矿中自俘获激子和自由激子与中间激子-声子耦合的相关性
低维卤化铅由于其作为单组分白光发射器的潜在应用而引起了越来越多的关注。这些材料表现出复杂的发射光谱结构，范围从自由激子窄带发射到自俘获激子宽带发射。然而，对于潜在的物理机制仍然没有达成共识，特别是在窄带和宽带发射的频谱中。在这里，我们的目的是阐明混合卤化物钙钛矿 BA 2 Pb(Br x Cl 1– x ) 4中发射光谱与激子-声子耦合之间的相关性。我们的研究结果表明，激子局域化和离域化之间的相互作用导致中间激子-声子耦合，导致自俘获激子的线形状超出黄-里斯模型。通过结合激子运动效应，我们建立了一个统一的光物理模型，描述从自陷激子型到自由激子型的发射光谱。这些结果为控制激子-声子相互作用的机制提供了重要的见解，并提供了控制二维钙钛矿白光发射的方法。
更新日期：2023-11-01
中文翻译：
二维混合卤化物钙钛矿中自俘获激子和自由激子与中间激子-声子耦合的相关性
低维卤化铅由于其作为单组分白光发射器的潜在应用而引起了越来越多的关注。这些材料表现出复杂的发射光谱结构，范围从自由激子窄带发射到自俘获激子宽带发射。然而，对于潜在的物理机制仍然没有达成共识，特别是在窄带和宽带发射的频谱中。在这里，我们的目的是阐明混合卤化物钙钛矿 BA 2 Pb(Br x Cl 1– x ) 4中发射光谱与激子-声子耦合之间的相关性。我们的研究结果表明，激子局域化和离域化之间的相互作用导致中间激子-声子耦合，导致自俘获激子的线形状超出黄-里斯模型。通过结合激子运动效应，我们建立了一个统一的光物理模型，描述从自陷激子型到自由激子型的发射光谱。这些结果为控制激子-声子相互作用的机制提供了重要的见解，并提供了控制二维钙钛矿白光发射的方法。
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