Nelson Jane C, Weichman Marissa L
Department of Chemistry, Princeton University, Princeton, New Jersey 08544, USA.
J Chem Phys. 2024 Aug 21;161(7). doi: 10.1063/5.0220077.
Gas-phase molecules are a promising platform to elucidate the mechanisms of action and scope of polaritons for optical control of chemistry. Polaritons arise from the strong coupling of a dipole-allowed molecular transition with the photonic mode of an optical cavity. There is mounting evidence of modified reactivity under polaritonic conditions; however, the complex condensed-phase environment of most experimental demonstrations impedes mechanistic understanding of this phenomenon. While the gas phase was the playground of early efforts in atomic cavity quantum electrodynamics, we have only recently demonstrated the formation of molecular polaritons under these conditions. Studying the reactivity of isolated gas-phase molecules under strong coupling would eliminate solvent interactions and enable quantum state resolution of reaction progress. In this Perspective, we contextualize recent gas-phase efforts in the field of polariton chemistry and offer a practical guide for experimental design moving forward.
气相分子是阐明用于化学光学控制的极化激元作用机制和范围的一个很有前景的平台。极化激元源于偶极允许的分子跃迁与光学腔光子模式的强耦合。有越来越多的证据表明在极化激元条件下反应活性会发生改变；然而，大多数实验演示中的复杂凝聚相环境阻碍了对这一现象的机理理解。虽然气相是早期原子腔量子电动力学研究的领域，但我们直到最近才证明在这些条件下分子极化激元的形成。研究强耦合下孤立气相分子的反应活性将消除溶剂相互作用，并能够对反应进程进行量子态分辨。在这篇展望文章中，我们将近期极化激元化学领域的气相研究置于背景中，并为未来的实验设计提供实用指南。
