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Giant strides in ultrashort laser pulse technology have enabled real-timeobservation of dynamical processes in complex molecular systems. Specifically,the discovery of oscillatory transients in the two-dimensional electronicspectra of photosynthetic systems stimulated a number of theoreticalinvestigations exploring possible physical mechanisms of the remarkable quantumefficiency of light harvesting processes. However, the theories employed havereached a high degree of sophistication and have become complex, making itdifficult to gain insights into microscopic processes and biologicallysignificant questions. In this work, we revisit the elementary aspects ofenvironment-induced fluctuations in the involved electronic energies andpresent a simple way to understand energy flow with the intuitive picture ofrelaxation in a funnel-type free-energy landscape. The presented free-energydescription of energy transfer reveals that typical photosynthetic systemsoperate in an almost barrierless regime. The approach also provides insightsinto the distinction between coherent and incoherent energy transfer andcriteria by which the necessity of the vibrational assistance is considered.

the journal of physical chemistry. b

Insights into photosynthetic energy transfer gained from free-energy  structure: Coherent transport, incoherent hopping, and vibrational assistance  revisited