2025/11/05 by Tichauer, Ruth H., Lednev, Maksim, Groenhof, Gerrit +1
#Chemical Physics (physics.chem-ph) #FOS: Physical sciences #Mesoscale and Nanoscale Physics (cond-mat.mes-hall) #Optics (physics.optics)
paper · doi:10.48550/arxiv.2511.03303
In the context of light-matter interactions between organic chromophores and confined photons of (plasmonic) nano-resonators, we introduce a general framework that couples ab initio QM/MM molecular dynamics with few-mode field quantization to simulate light-matter interactions of molecular emitters at the nanoscale. Arbitrary, lossy, and spatially inhomogeneous photonic environments are represented by a minimal set of interacting modes fitted to their spectral density, while geometry-dependent molecular properties are computed on the fly. Applications to few-molecule strong coupling show that strong coupling persists when molecular degrees of freedom and disorder are included for the chosen system consisting of a nanoparticle dimer coupled to multiple emitters. At the same time, symmetry-protected degeneracies of two-level models are lifted. The framework further reveals how spatial field inhomogeneity and molecular disorder shape cavity-mediated energy transfer, illustrated for an HBQ-Methylene Blue donor-acceptor combination in a five-emitter system.