Kavli Affiliate: Graham R. Fleming
| First 5 Authors: Akihito Ishizaki, Graham R. Fleming, , ,
| Summary:
Giant strides in ultrashort laser pulse technology have enabled real-time
observation of dynamical processes in complex molecular systems. Specifically,
the discovery of oscillatory transients in the two-dimensional electronic
spectra of photosynthetic systems stimulated a number of theoretical
investigations exploring possible physical mechanisms of the remarkable quantum
efficiency of light harvesting processes. However, the theories employed have
reached a high degree of sophistication and have become complex, making it
difficult to gain insights into microscopic processes and biologically
significant questions. In this work, we revisit the elementary aspects of
environment-induced fluctuations in the involved electronic energies and
present a simple way to understand energy flow with the intuitive picture of
relaxation in a funnel-type free-energy landscape. The presented free-energy
description of energy transfer reveals that typical photosynthetic systems
operate in an almost barrierless regime. The approach also provides insights
into the distinction between coherent and incoherent energy transfer and
criteria by which the necessity of the vibrational assistance is considered.
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