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arXiv · 1609.01520

Multiple Rabi Splittings under Ultra-Strong Vibrational Coupling

Jino George·Thibault Chervy·Atef Shalabney·Eloïse Devaux·Hidefumi Hiura·Cyriaque Genet·Thomas W. Ebbesen
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Abstract

From the high vibrational dipolar strength offered by molecular liquids, we demonstrate that a molecular vibration can be ultra-strongly coupled to multiple IR cavity modes, with Rabi splittings reaching $24\%$ of the vibration frequencies. As a proof of the ultra-strong coupling regime, our experimental data unambiguously reveal the contributions to the polaritonic dynamics coming from the anti-resonant terms in the interaction energy and from the dipolar self-energy of the molecular vibrations themselves. In particular, we measure the opening of a genuine vibrational polaritonic bandgap of ca. $60$ meV. We also demonstrate that the multimode splitting effect defines a whole vibrational ladder of heavy polaritonic states perfectly resolved. These findings reveal the broad possibilities in the vibrational ultra-strong coupling regime which impact both the optical and the molecular properties of such coupled systems, in particular in the context of mode-selective chemistry.

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Jino George, Thibault Chervy, Atef Shalabney, Eloïse Devaux, Hidefumi Hiura, Cyriaque Genet, Thomas W. Ebbesen. 2016-09-06. Multiple Rabi Splittings under Ultra-Strong Vibrational Coupling. https://doi.org/10.1103/physrevlett.117.153601

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