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多模腔中高度失谐光子模式的强耦合诱导频移

Strong coupling-induced frequency shifts of highly detuned photonic modes in multimode cavities.

作者信息

Thomas Philip A, Barnes William L

机构信息

Department of Physics and Astronomy, University of Exeter, Exeter EX4 4QL, United Kingdom.

出版信息

J Chem Phys. 2024 May 28;160(20). doi: 10.1063/5.0208379.

Abstract

Strong coupling between light and molecules is a fascinating topic exploring the implications of the hybridization of photonic and molecular states. For example, many recent experiments have explored the possibility that strong coupling of photonic and vibrational modes might modify chemical reaction rates. In these experiments, reactants are introduced into a planar cavity, and the vibrational mode of a chemical bond strongly couples to one of the many photonic modes supported by the cavity. Some experiments quantify reaction rates by tracking the spectral shift of higher-order cavity modes that are highly detuned from the vibrational mode of the reactant. Here, we show that the spectral position of these cavity modes, even though they are highly detuned, can still be influenced by strong coupling. We highlight the need to consider this strong coupling-induced frequency shift of cavity modes if one is to avoid underestimating cavity-induced reaction rate changes. We anticipate that our work will assist in the re-analysis of several high-profile results and has implications for the design of future strong coupling experiments.

摘要

光与分子之间的强耦合是一个引人入胜的课题,它探索了光子态与分子态杂化的影响。例如,最近的许多实验都探讨了光子与振动模式的强耦合可能改变化学反应速率的可能性。在这些实验中,将反应物引入平面腔中,化学键的振动模式与腔所支持的众多光子模式之一强烈耦合。一些实验通过跟踪与反应物振动模式高度失谐的高阶腔模式的光谱位移来量化反应速率。在这里,我们表明,即使这些腔模式高度失谐,它们的光谱位置仍然会受到强耦合的影响。我们强调,如果要避免低估腔诱导的反应速率变化,就需要考虑这种由强耦合引起的腔模式频移。我们预计,我们的工作将有助于对几个备受瞩目的结果进行重新分析,并对未来强耦合实验的设计产生影响。

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