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Nonlinear spectroscopy has revealed long-lasting oscillations in the opticalresponse of a variety of photosynthetic complexes. Different theoretical modelswhich involve the coherent coupling of electronic (excitonic) orelectronic-vibrational (vibronic) degrees of freedom have been put forward toexplain these observations. The ensuing debate concerning the relevance ofeither one or the other mechanism may have obscured their potential synergy. Toillustrate this synergy, we quantify how the excitonic delocalization in theLH2 unit of Rhodopseudomonas Acidophila purple bacterium, leads to correlationsof excitonic energy fluctuations, relevant coherent vibronic coupling and,importantly, a decrease in the excitonic dephasing rates. Combining theseeffects, we identify a feasible origin for the long-lasting oscillationsobserved in fluorescent traces from time-delayed two-pulse single moleculeexperiments performed on this photosynthetic complex.

On the theory of excitonic delocalization for robust vibronic dynamics in LH2