Vibrational polaritons is an intensely studied new research topic because of the potential for controlling the spectroscopy and chemical reactions of molecules and materials through their coupling to confined infrared fields. Recent experiments have demonstrated that polariton spectra depend on the shape of dipole moment function of the molecular mode. Here, we use the multi-level quantum Rabi (MLQR) model to find the polariton spectrum of a molecular mode, modeled by a Morse oscillator, coupled to an infrared cavity mode. We show that in the strong and ultrastrong coupling regime the structure of the polariton spectrum is strongly determined by the type of polar molecular species. In addition, we apply the same theory to describe successfully ultrafast polariton-to-polariton transitions in two-dimensional infrared and pump-probe spectroscopy of a hybrid system formed by coupling the NO band of sodium nitroprusside to an infrared cavity. Our work offers mechanistic insights on spectroscopy and chemistry of vibrational polariton states.

Non-linear spectroscopy of anharmonic vibrational polaritons in the strong and ultrastrong coupling regime

ACS Fall 2021

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