Multilayer-MCTDH approach to the energy transfer dynamics in the LH2 antenna complex

Abstract

The multilayer multiconfiguration time-dependent Hartree method is used to study the coupled exciton–vibrational dynamics in a high-dimensional nonameric model of the LH2 antenna complex of purple bacteria. The exciton–vibrational coupling is parametrized within the Huang–Rhys model according to phonon and intramolecular vibrational modes derived from an experimental bacteriochlorophyll spectral density. In contrast to reduced density matrix approaches, the Schrödinger equation is solved explicitly, giving access to the full wave function. This facilitates an unbiased analysis in terms of the coupled dynamics of excitonic and vibrational degrees of freedom. For the present system, we identify spectator modes for the B800 to B800 transfer and we find a non-additive effect of phonon and intramolecular vibrational modes on the B800 to B850 exciton transfer.