Optical Cavity Manipulation and Nonlinear UV Molecular Spectroscopy of Conical Intersections in Pyrazine

초록

Optical cavities provide a versatile platform for manipulating the excited-state dynamics of molecules via stronglight-matter coupling. We employ optical absorption and two-multidimensional electronic spectroscopy simulations to investigatethe effect of optical cavity coupling in the nonadiabatic dynamics ofphotoexcited pyrazine. We observe the emergence of a novelpolaritonic conical intersection (PCI) between the electronic darkstate and photonic surfaces as the cavity frequency is tuned. The PCIcould significantly change the nonadiabatic dynamics of pyrazine bydoubling the decay rate constant of the S2state population. Moreover, the absorption spectrum and excited-state dynamics could besystematically manipulated by tuning the strong light-matter interaction, e.g., the cavity frequency and cavity coupling strength. We propose that a tunable optical cavity-molecule system may provide promising approaches for manipulating the photophysical properties of molecules

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