Strong coupling beyond the light-line (dataset)
Menghrajani, K; Barnes, WL
Date: 27 August 2020
Publisher
University of Exeter
Publisher DOI
Abstract
Strong coupling of molecules placed in an optical microcavity may lead to the formation of hybrid states called polaritons; states that inherit characteristics of both the optical cav- ity modes and the molecular resonance. Developing a better understanding of the matter characteristics of these hybrid states has been the focus of much ...
Strong coupling of molecules placed in an optical microcavity may lead to the formation of hybrid states called polaritons; states that inherit characteristics of both the optical cav- ity modes and the molecular resonance. Developing a better understanding of the matter characteristics of these hybrid states has been the focus of much recent attention. Here, as we will show, a better understanding of the role of the optical modes supported by typical cavity structures is also required. Typical microcavities used in molecular strong coupling experiments support more than one mode at the frequency of the material resonance, but previous work has almost exclusively considered only one of these modes. Many experiments involving strong coupling make use of metal-clad microcavities, ones with metallic mirrors. Metal-clad microcavities are well known to support coupled plasmon modes in addition to the standard microcavity mode. However, the coupled plasmon modes associated with a metal-clad optical microcavity lie beyond the light-line and are thus not probed in typical experiments on strong coupling. Here we investigate, through experiment and numerical modelling, the interaction between molecules within a cavity and the modes both inside and outside the light-line. Making use of grating coupling and a metal-clad microcavity we pro- vide an experimental demonstration that such modes undergo strong coupling. We further show that a common variant of the metal-clad microcavity, one in which the metal mirrors are replaced by distributed Bragg reflector also show strong coupling to modes that exist in these structures beyond the light-line. Our results highlight the need to consider the effect of beyond the light-line modes on the strong coupling of molecular resonances in microcavities, and may be of relevance in designing strong coupling resonators for chemistry and materials science investigations.
Physics and Astronomy
Faculty of Environment, Science and Economy
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