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Investigating the collective nature of cavity-modified chemical kinetics under vibrational strong coupling
Nanophotonics ( IF 7.5 ) Pub Date : 2024-03-18 , DOI: 10.1515/nanoph-2024-0026
Lachlan P. Lindoy 1 , Arkajit Mandal 1 , David R. Reichman 1
Affiliation  

In this paper, we develop quantum dynamical methods capable of treating the dynamics of chemically reacting systems in an optical cavity in the vibrationally strong-coupling (VSC) limit at finite temperatures and in the presence of a dissipative solvent in both the few and many molecule limits. In the context of two simple models, we demonstrate how reactivity in the collective VSC regime does not exhibit altered rate behavior in equilibrium but may exhibit resonant cavity modification of reactivity when the system is explicitly out of equilibrium. Our results suggest experimental protocols that may be used to modify reactivity in the collective regime and point to features not included in the models studied, which demand further scrutiny.

中文翻译:

研究振动强耦合下空腔改性化学动力学的集体性质

在本文中,我们开发了量子动力学方法,能够在有限温度下以及在少分子和多分子中存在耗散溶剂的情况下,在振动强耦合(VSC)极限下处理光腔中化学反应系统的动力学限制。在两个简单模型的背景下,我们演示了反应性如何集体VSC 状态在平衡状态下不会表现出速率行为的改变,但当系统明显脱离平衡时,可能会表现出反应性的谐振腔变化。我们的结果提出了可用于修改集体制度中的反应性的实验方案,并指出了所研究模型中未包含的特征,这些特征需要进一步审查。
更新日期:2024-03-18
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