Elucidation of near-resonance vibronic coherence lifetimes by nonadiabatic electronic-vibrational state character mixing

摘要: Recent work suggests that the long-lived coherences observed in both natural and artificial light-harvesting systems (such as Fenna–Matthews–Olson complex) could be attributed to mixing of pigments’ electronic vibrational degrees freedom. To investigate underlying mechanism these long coherence lifetimes, a sophisticated description interactions between molecular aggregates nonequilibrium fluctuations surrounding environment is necessary. This done by implementing hierarchical equations motion approach on model homodimers, method used intermediate coupling regime for many wherein phonons play nontrivial roles exciton dynamics. Here we report character change vibronic states—reflective property states—induced an interplay system parameters within exciton-vibrational near-resonance regime. dictates vital aspects lifetime; tracking degree mixing, are able elucidate relationship lifetime energy fluctuation relaxation dephasing pathways.