Origin of long-lived coherence and excitation dynamics in pigment-protein complexes

TL;DR

This paper investigates how discrete vibrational modes in pigment-protein complexes enhance long-lived quantum coherence and facilitate efficient energy transfer, combining analytical estimates with detailed system studies.

Contribution

It introduces a theory linking vibrational coherence to long-lived excitonic coherence, supported by detailed analysis of energy transfer dynamics in pigment-protein complexes.

Findings

Vibrational modes weaken exciton-environment interactions.

Ground-state vibrational coherence persists long and aids energy transfer.

Nonequilibrium effects promote exciton migration.

Abstract

We explore the mechanism for the long-lived quantum coherence by considering the discrete phonon modes: these vibrational modes effectively weaken the exciton-environment interaction, due to the new composite (polaron) formed by excitons and vibrons. This subsequently demonstrates the role of vibrational coherence which greatly contributes to long-lived feature of the excitonic coherence that has been observed in femtosecond experiments. The estimation of the timescale of coherence elongated by vibrational modes is given in an analytical manner. To test the validity of our theory, we study the pigment-protein complex in detail by exploring the energy transfer and coherence dynamics. The ground-state vibrational coherence generated by incoherent radiations is shown to be long-survived and is demonstrated to be significant in promoting the excitation energy transfer. This is attributed to the nonequilibriumness of the system caused by the detailed-balance-breaking, which funnels the downhill migration of excitons.