Vibrational strong coupling (VSC) is emerging as a powerful tool for controlling the physical and chemical properties of molecules and materials. [1] It involves the coupling of a specific vibrational mode to a confined infrared photon in a Fabry-Perot cavity. In this study, we investigated the modification of oscillator strength of an asymmetric stretching band of CS2 molecules under ultra-strong coupling condition. [2] We experimentally proved this by taking the area ratio of asymmetric stretching and combination band by selectively coupling the former. Under cavity conditions, a non-linear enhancement in the area ratio was observed upon varying the coupling strength. Whereas no such variations in the area ratio happened for bare molecules. This implies a non-linear increase in the self-interaction of vibrational transition dipole of the asymmetric stretching band under coupling conditions. This is explained by a quantum mechanical model that predicts quadratic behaviour under ultra-strong coupling conditions.

Boosting Self-interactions of Molecular Vibrations under Ultra-Strong Coupling Conditions

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27th CRSI National Symposium in Chemistry

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