Disorder-induced non-Gaussian states in large ensembles of cavity-coupled molecules

We analyze vibrational dynamics in a toy model for polaritonic chemistry under collective electronic strong coupling. In a Holstein-Tavis-Cummings model, incoherently excited by a photon, we show that disorder leads to non-Gaussian states of vibrational modes on short time scales at the single-molecule level. Using exact matrix product state simulations, we demonstrate that this effect can remain robust for larger molecule numbers, implying that nuclear wave packets cannot be effectively described by thermal states. Furthermore, we compare simulations of the exact quantum dynamics with semiclassical approximations. We find that the Ehrenfest approximation can only well reproduce ensemble-averaged observables for very large system sizes. Also simulations in the truncated Wigner approximation fail to capture the non-Gaussian effects. Our work highlights the importance of disorder and genuine quantum effects in cavity-modified nuclear dynamics in polaritonic chemistry.

Source: arXiv:2604.18456v1 - http://arxiv.org/abs/2604.18456v1 PDF: https://arxiv.org/pdf/2604.18456v1 Original Link: http://arxiv.org/abs/2604.18456v1