Quantum dynamics of the photoisomerization of a single thiacynine iodide molecule embedded in an optical microcavity was theoretically studied. The molecular model consisting of two electronic states and the reaction coordinate was coupled to a single cavity mode via the quantum Rabi Hamiltonian. We show that an electronic excitation of the molecule at cis configuration is followed by the generation of two photons in the trans configuration upon nonadiabatic isomerization. Although conditions for this phenomenon to operate in the collective strong light-matter coupling regime were found to be unfeasible for the present system, our finding suggests a new mechanism that, without ultrastrong coupling, achieves photon down-conversion by exploiting the emergent molecular dynamics arising in polaritonic architectures.
Strong coupling (SC) between light and matter has emerged in the last decade as a promising tool to control room-temperature photophysical processes in organic molecules. In this article, we aim to provide a pedagogical introduction to the various flavors of molecular SC involving (a) a single molecule in an optical nanocavity (e.g. a plasmonic junction), and (b) many molecules in an optical microcavity (the collective regime). Although the linear optical properties of these two systems are very similar, their chemical dynamics are drastically different from each another. We will highlight the relevant timescales and rates that can be manipulated via both flavors of SC. We will illustrate these ideas with theoretical and experimental examples from our previous work, which will help us distill the physical mechanisms that are at play in each SC case.
Access to the requested content is limited to institutions that have purchased or subscribe to SPIE eBooks.
You are receiving this notice because your organization may not have SPIE eBooks access.*
*Shibboleth/Open Athens users─please
sign in
to access your institution's subscriptions.
To obtain this item, you may purchase the complete book in print or electronic format on
SPIE.org.
INSTITUTIONAL Select your institution to access the SPIE Digital Library.
PERSONAL Sign in with your SPIE account to access your personal subscriptions or to use specific features such as save to my library, sign up for alerts, save searches, etc.