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Boosting self-interaction under USC_ChemrXiv.pdf (4.52 MB)

Boosting Self-interaction of Molecular Vibrations under Ultra-strong Coupling Condition

submitted on 19.02.2021, 08:18 and posted on 22.02.2021, 05:18 by Akhila Kadyan, Anil Shaji, Jino George
In this letter, we investigated the modification of oscillator strength of an asymmetric stretching band of CS2 by strong coupling to an infrared cavity photon. This is achieved by placing liquid CS2 in a Fabry-Perot resonator and tune the cavity mode position to match with the molecular vibrational transition. Ultra-strong coupling improves the self-interaction of transition dipoles of asymmetric stretching band of CS2 that resulted in an increase of its own oscillator strength. We experimentally proved this by taking the area ratio of asymmetric stretching and combination band by selectively coupling the former one. A non-linear increase in the oscillator strength of the asymmetric stretching band is observed upon varying the coupling strength. This is explained by a quantum mechanical model that predicts quadratic behavior under ultra-strong coupling condition. These findings will set up a new paradigm for understanding chemical reaction modification by vacuum field coupling.


DST-SERB, Core Research Grant (EMR/2017/003455)

MHRD-Scheme for Transformational and Advanced Research in Sciences (STARS 175/2019)

DST-SERB, Core Research Grant EMR/2016/007221

QuEST program of DST through project No. Q113 under Theme 4


Email Address of Submitting Author


IISER Mohali



ORCID For Submitting Author


Declaration of Conflict of Interest

The authors declare no competing financial interests.