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Coherent Light Harvesting through Strong Coupling to Confined Light.

ABSTRACT: When photoactive molecules interact strongly with confined light modes, new hybrid light-matter states may form: the polaritons. These polaritons are coherent superpositions of excitations of the molecules and of the cavity photon. Recently, polaritons were shown to mediate energy transfer between chromophores at distances beyond the Förster limit. Here we explore the potential of strong coupling for light-harvesting applications by means of atomistic molecular dynamics simulations of mixtures of photoreactive and non-photo-reactive molecules strongly coupled to a single confined light mode. These molecules are spatially separated and present at different concentrations. Our simulations suggest that while the excitation is initially fully delocalized over all molecules and the confined light mode, it very rapidly localizes onto one of the photoreactive molecules, which then undergoes the reaction.

SUBMITTER: Groenhof G

PROVIDER: S-EPMC6129961 | biostudies-literature | 2018 Sep

REPOSITORIES: biostudies-literature

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Coherent Light Harvesting through Strong Coupling to Confined Light.

Groenhof Gerrit G Toppari J Jussi JJ

The journal of physical chemistry letters 20180813 17

When photoactive molecules interact strongly with confined light modes, new hybrid light-matter states may form: the polaritons. These polaritons are coherent superpositions of excitations of the molecules and of the cavity photon. Recently, polaritons were shown to mediate energy transfer between chromophores at distances beyond the Förster limit. Here we explore the potential of strong coupling for light-harvesting applications by means of atomistic molecular dynamics simulations of mixtures o ...[more]

PMID: 30085671

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Project description: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 cavity 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. While the effect of strong coupling to multiple photonic modes has been considered before, here we extend this topic by looking at strong coupling between one vibrational mode and multiple photonic 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 modeling, 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 provide 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.

Dataset Information

Coherent Light Harvesting through Strong Coupling to Confined Light.

Publications

Coherent Light Harvesting through Strong Coupling to Confined Light.

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