Speaker
Description
Vibrational strong coupling, i.e. the formation of polaritons between the vacuum field in Fabry Perot cavities and molecular vibrations, is discussed to allow tuning and steering chemical reactivity. However, mechanistic insights into the vibrational dynamics of the formed vibropolaritons, specifically from experiments, are still limited and not yet available for organic molecules, which are relevant in many synthesis applications.
We have started to perform 2D-IR spectroscopy on organic molecules in cavities inspired by some of the pioneering 2D-IR studies on coordination complexes under VSC, upon solving a lot of experimental constraints.
2D-IR spectra reveal vibrational dynamics of the polaritonic states and couplings between contributing states. We are able to report lifetimes of polaritons for selected organic molecules and observe strong modulation of those in comparison to the uncoupled molecules by the cavity. We find that 2D-IR spectra of vibropolaritons, comprised of signals from the cavity, the bare molecules beside the lower and upper polaritons are more and more complex to analyze the shorter the vibrational lifetime of the oscillator under investigation is.