Journal of Chemical Physics, Vol.108, No.18, 7763-7774, 1998
Exciton-migration and three-pulse femtosecond optical spectroscopies of photosynthetic antenna complexes
A theory for four-wave-mixing signals from molecular aggregates, which includes effects of two-exciton states, static disorder, and coupling to a phonon bath with an arbitrary spectral density, is developed. The third-order polarization is rigorously partitioned into a coherent and a sequential contribution. The latter is given by a sum of an exciton-hopping and a ground state (bleaching) terms, both expressed using the doorway-window representation. Applications are made to photon-echo and pump-probe spectroscopies of the B850 system of the LH2 antenna in purple bacteria.
Keywords:LIGHT-HARVESTING COMPLEX;RHODOBACTER-SPHAEROIDES;RHODOPSEUDOMONAS-ACIDOPHILA;EXCITATION TRANSFER;ENERGY-TRANSFER;B850 ANTENNA;MOLECULES;BACTERIA;DYNAMICS