Speaker
Description
Polaritonic chemistry bears the potential to tune molecular properties and steer chemical reactions by direct and controlled manipulation of strong light-matter interactions1, i.e. vibropolaritons formed under vibrational strong coupling (VSC) between the confined electromagnetic field in Fabry Perot cavities and molecular modes. However, experimental insights into the fundamental mechanisms and dynamics of vibropolaritons and implications for systematically tuning chemistry are still debated or lacking and difficult to obtain.
We aim to utilize coherent multidimensional vibrational spectroscopy (2D-IR) to study the ultrafast dynamics of vibropolaritions, with organic molecules. 2D-IR spectra can access vibrational lifetimes, couplings and energy transfer processes and how these are modulated upon formation of the delocalized hybrid states in contrast to pure molecular states. We have successfully established the experimental protocol to perform 2D-IR of vibropolaritons of carbonyl modes in organic molecules. These vibrational modes have a much shorter lifetime than previously studied inorganic complexes (i.e. W(CO)6)2 , hampering analysis of data as cavity contributions, rabi oscillations and spectra of uncoupled molecules all contribute to the observed data. However, first analysis shows presence of cross peaks between lower and upper polarition with dynamic features differing from the bare molecules.
References
[1] Thomas, A. et al., Tilting a Ground-State Reactivity Landscape by Vibrational Strong Coupling, Science 2019, 363 (6427), 615–619
[2] Xiang, B. et al., Intermolecular Vibrational Energy Transfer Enabled by Microcavity Strong Light–Matter Coupling, Science 2020, 368 (6491), 665–667.