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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.
Juan Perez andJoel Yuen-Zhou
"Polariton assisted down-conversion of photons via nonadiabatic molecular dynamics", Proc. SPIE 11464, Physical Chemistry of Semiconductor Materials and Interfaces XIX, 114640P (20 August 2020); https://doi.org/10.1117/12.2569308
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Juan Perez, Joel Yuen-Zhou, "Polariton assisted down-conversion of photons via nonadiabatic molecular dynamics," Proc. SPIE 11464, Physical Chemistry of Semiconductor Materials and Interfaces XIX, 114640P (20 August 2020); https://doi.org/10.1117/12.2569308