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In most theoretical descriptions of collective strong coupling of organicmolecules to a cavity mode, the molecules are modeled as simple two-levelsystems. This picture fails to describe the rich structure provided by theirinternal rovibrational (nuclear) degrees of freedom. We investigate afirst-principles model that fully takes into account both electronic andnuclear degrees of freedom, allowing an exploration of the phenomenon of strongcoupling from an entirely new perspective. First, we demonstrate thelimitations of applicability of the Born-Oppenheimer approximation in stronglycoupled molecule-cavity structures. For the case of two molecules, we also showhow dark states, which within the two-level picture are effectively decoupledfrom the cavity, are indeed affected by the formation of collective strongcoupling. Finally, we discuss ground-state modifications in the ultra-strongcoupling regime and show that some molecular observables are affected by thecollective coupling strength, while others only depend on the single-moleculecoupling constant.

Cavity-induced modifications of molecular structure in the strong coupling regime