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极化激元发光中电子-振动相互作用的影响:非马尔可夫范诺共振与热发光

Effects of Electron-Vibration Interaction in Polariton Luminescence: Non-Markovian Fano Resonances and Hot Luminescence.

作者信息

Fainberg B D, Osipov V Al

机构信息

Faculty of Sciences, Holon Institute of Technology, 52 Golomb Street, Holon 5810201, Israel.

School of Chemistry, Tel-Aviv University, Tel-Aviv 69978, Israel.

出版信息

J Phys Chem A. 2022 May 12;126(18):2761-2777. doi: 10.1021/acs.jpca.1c10405. Epub 2022 Apr 28.

Abstract

We have developed a non-Markovian theory of the polariton luminescence taking the molecular vibrations into account. The calculations were performed in the polariton basis. We have shown that the frequency shift and the polariton spectral line broadening strongly depend on the frequency-dependent exciton contribution to the polariton. In the single-mode microcavity, our non-Markovian theory predicts the Fano resonances in the polariton luminescence and also narrowing of the spectral lines with the increase of the total number of molecules in the case of the intramolecular nature of the low-frequency vibrations. The theory enables us to consider a nonequilibrium (hot) exciton-polariton luminescence similar to the hot luminescence of molecules and crystals. This opens a way for its observation in organic-based nanodevices.

摘要

我们已经发展了一种考虑分子振动的极化激元发光的非马尔可夫理论。计算是在极化激元基矢下进行的。我们已经表明,频移和极化激元谱线展宽强烈依赖于频率相关的激子对极化激元的贡献。在单模微腔中,我们的非马尔可夫理论预测了极化激元发光中的法诺共振,并且在低频振动具有分子内性质的情况下,随着分子总数的增加谱线变窄。该理论使我们能够考虑类似于分子和晶体的热发光的非平衡(热)激子 - 极化激元发光。这为在有机基纳米器件中对其进行观测开辟了一条途径。

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