Abstract

Vibrational strong coupling provides a convenient way to modify the energy of molecular vibrations and to explore the control of chemical reactivity. In this work, we theoretically report the various vibrational anharmonicities that modulate the dynamics of optomechanically coupled W(CO)6-cavity. The optomechanical free-space cavity consists of movable photonic crystal membrane, which creates photonic bound states to interact with the molecular vibration. This coupled system is used for realizing strong optomechanical dispersive or dissipative type coupling, which provides a platform to explore the new regimes of optomechanical interaction. The addition of different strong coupling and mechanical (nuclear) anharmonicities to the optical cavity establishes a modified splitting dynamics in the absorption spectrum and shows that the ground-state bleach of coupled W(CO)6-cavity has a broad, multisigned spectral response. This work demonstrates the possibility of systematic and predictive modification of the multimode spectroscopy of optomechanical W(CO)6-cavity polariton system.

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