Lindoy Lachlan P, Mandal Arkajit, Reichman David R
Columbia University, 3000 Broadway, New York, NY, USA.
Nanophotonics. 2024 Mar 18;13(14):2617-2633. doi: 10.1515/nanoph-2024-0026. eCollection 2024 Jun.
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 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.
在本文中，我们开发了量子动力学方法，该方法能够在有限温度下以及存在耗散溶剂的情况下，在少分子和多分子极限下，处理处于振动强耦合（VSC）极限的光学腔中化学反应系统的动力学。在两个简单模型的背景下，我们展示了在VSC regime中，反应性在平衡时不会表现出速率行为的改变，但当系统明显处于非平衡状态时，可能会表现出反应性的共振腔修饰。我们的结果提出了可用于在集体 regime中改变反应性的实验方案，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。
