Vibrational strong coupling (VSC) generates hybridized quasiparticles of molecular vibrational and cavity electromagnetic modes, known as molecular vibrational polaritons (MVPs). VSC has arisen as a promising handle to manipulate chemical reactions in condensed phases. Extensive experimental evidence has shown that, simply by placing a solution inside an optical cavity, the reaction rate can be either accelerated or decelerated by VSC, and the reaction selectivity can also be altered. Polaritons, as light-matter coupled systems, are examples how molecular properties can be changed by coupling. However the exact mechanism of polariton chemistry remain elusive. We aim to understand it by using two-dimensional infrared (2D IR) spectroscopy to study the ultrafast dynamics of molecular vibrational polaritons, and to advance our control in condensed phase chemistry and develop new quantum information technology platforms.
One focus is to monitor ultrafast dynamical processes in MVPs, such as energy transfer and the modification of chemical dynamics. Our research involves using pump probe and 2D IR spectroscopies to study how MVPs will alter certain chemical reaction rates and affect the ultrafast dynamics of chemical systems. We found that MVPs can modify vibrational energy dynamics, such as intermolecular energy transfer, and create hot vibrational modes.
We also develop quantum technology platforms with molecular vibrational polaritons. Since they inherit nonlinearity from the molecule and delocalization from the photon, MVPs show potential to serve as quantum bits for quantum information technology under room temperature. We have realized various quantum states and coherences of polariton systems, and visualized coherence transfer in a simulation platform.