Simulation of Femtosecond Phase-Locked Double-Pump Signals of Individual Light-Harvesting Complexes LH2

Recent phase-locked femtosecond double-pump experiments on individual light-harvesting complexes LH2 of purple bacteria at ambient temperature revealed undamped oscillatory responses on a time scale of at least 400 fs [ Hildner et al. Science 2013, 340, 1448 ]. Using an excitonic Hamiltonian for LH2 available in the literature, we simulate these signals numerically by a method that treats excitonic couplings and exciton-phonon couplings in a nonperturbative manner. The simulations provide novel insights into the origin of coherent dynamics in individual LH2 complexes.