Interplay between disorder, local relaxation, and collective behavior for an ensemble of emitters outside versus inside a cavity
Interplay between disorder, local relaxation, and collective behavior for an ensemble of emitters outside versus inside a cavity
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空腔外部和内部的发射体整体的无序、局部松弛和集体行为之间的相互作用
DOI：
10.1103/physreva.108.023708
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发表时间：
2023
影响因子：
2.9
通讯作者：
Nitzan, Abraham
中科院分区：
文献类型：
--
作者：
Zhou, Zeyu;Chen, Hsing-Ta;Subotnik, Joseph E.;Nitzan, Abraham
使用简单有效的哈密顿量来研究单模腔内部和外部的两级发射器的集合，集体光学响应与分子静态和动态无序之间的相互作用。我们通过随机调节分子跃迁频率以及发射器与电磁场之间的耦合来模拟环境紊乱。我们还考虑分子间相互作用和定向障碍的影响。我们研究这些效应如何导致稳态吸收（腔外）、透射光谱（腔内）和局部分子过程（例如单分子反应）的产率的新特征。在腔外，集体行为表现为稳态吸收的线宽、发射光谱和局部化学产率。然而，在空腔内部，集体行为主要决定拉比分裂。还研究了定向障碍下分子间相互作用的影响。在大多数情况下，对于所有类型的紊乱，如果我们增加紊乱，我们会发现分子反应的集体性质减少（较小的有效），因此拉比分裂收缩会随着定向紊乱而发生。此外，我们发现静态无序比动态无序对集体行为更具破坏性。
The interplay between collective optical response and molecular static and dynamic disorder is studied using simple effective Hamiltonians for an ensemble of two-level emitters inside and outside a single-mode cavity. We model environmental disorder by randomly modulating the molecular transition frequencies and the coupling between the emitters and the electromagnetic field. We also consider the effects of intermolecular interactions and orientational disorder. We investigate how these effects lead to new features in the steady-state absorption (outside the cavity), transmission spectra (inside the cavity), and the yield of local molecular processes such as a unimolecular reaction. Outside the cavity, the collective behavior is manifested in the linewidth of the steady-state absorption, the emission spectrum, and the local chemical yield. Inside the cavity, however, the collective behavior primarily determines the Rabi splitting. The effects of intermolecular interactions under orientational disorder are also studied. For the most part, for all types of disorder, if we increase disorder, we find a reduction in the collective nature of the molecular response (smaller effective) and therefore the Rabi splitting contraction occurs with orientational disorder. Moreover, we find that static disorder is more destructive to collective behavior than dynamic disorder.
影响因子：
64.8
作者：
Yoshie, T;Scherer, A;Deppe, DG
通讯作者：
Deppe, DG
影响因子：
10.8
作者：
Mayte Gómez-Castaño;Andrés Redondo-Cubero;Lionel Buisson;Jose Luis Pau;A. Mihi;Serge Ravaine;R. Vallée;Abraham Nitzan;M. Sukharev
通讯作者：
Mayte Gómez-Castaño;Andrés Redondo-Cubero;Lionel Buisson;Jose Luis Pau;A. Mihi;Serge Ravaine;R. Vallée;Abraham Nitzan;M. Sukharev
分子发射功率谱理论。
DOI：
10.1063/5.0027796
发表时间：
2020
期刊：
The Journal of chemical physics
影响因子：
--
作者：
Siwei Wang;Ming;Yi;G. Scholes;Liang
通讯作者：
Liang