Strong Coupling in Infrared Plasmonic Cavities

J Phys Chem Lett. 2022 Oct 20;13(41):9673-9678. doi: 10.1021/acs.jpclett.2c02304. Epub 2022 Oct 10.

Abstract

Controlling molecular spectroscopy and even chemical behavior in a cavity environment is a subject of intense experimental and theoretical interest. In Fabry-Pérot cavities, strong (radiation-matter) coupling phenomena without an intense radiation field often rely on the number of chromophore molecules collectively interacting with a cavity mode. For plasmonic cavities, the cavity field-matter coupling can be strong enough to manifest strong coupling involving even a single molecule. To this end, infrared plasmonic cavities can be particularly useful in understanding vibrational strong coupling. Here we present a procedure for estimating the radiation-matter coupling and, equivalently, the mode volume as well as the mode lifetime and quality factor for plasmonic cavities of arbitrary shapes and use it to estimate these quantities for infrared cavities of two particularly relevant geometries comprising several n-doped semiconductors. Our calculations demonstrate very high field confinement and low mode volumes of these cavities despite having relatively low quality factors, which is often the case for plasmonic cavities.