Molecular polaritons created by the strong coupling between matter and field in microcavities enable the control of molecular dynamical processes and optical response. Multidimensional infrared spectroscopy is proposed for monitoring the polariton-assisted cooperative properties. The response of molecules to local fluctuations is incorporated and the full dynamics is monitored through the time- and frequency-resolved multidimensional signal. The cooperativity against solvent-induced disorder and its connection to the localization of the vibrational excitations are predicted. New insights are provided for recent 2DIR experiments on vibrational polaritons.
J Phys Chem Lett
- 0306 Physical Chemistry (incl. Structural)