Exciton−Vibrational Relaxation and Transient Absorption Dynamics in LH1 of Rhodopseudomonas viridis:  A Redfield Theory Approach

Autor: Novoderezhkin, V., Grondelle, R. van
Zdroj: The Journal of Physical Chemistry - Part B; June 2002, Vol. 106 Issue: 23 p6025-6037, 13p
Abstrakt: We explain the ultrafast transient absorption (TA) dynamics in the core LH1 antenna of Rhodopseudomonas viridis at 77 K (Monshouwer, R.; Baltuška, A.; van Mourik, F.; van Grondelle, R. J. Phys. Chem. A 1998, 102, 4360) using a disordered exciton model with strong coupling to two vibrational modes and weak coupling of vibrational and electronic coordinates to the thermal bath. A quantitative fit of the excitation wavelength- dependent TA dynamics was obtained using the density matrix equation with the Redfield relaxation operator. The sequential and coherent contributions to the TA dynamics were analyzed separately. The time-dependent red shift of TA was explained in terms of exciton relaxation. The lifetimes of higher exciton states of 12−75 fs (depending on the state) were determined from the fit.
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