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The role of resonant nuclear modes in vibrationally assisted energy transport: The LHCII complex

Pallavi Bhattacharyya, Graham R. Fleming

2020The Journal of Chemical Physics23 citationsDOIOpen Access PDF

Abstract

In this paper, we discuss the explicit role of resonant nuclear/vibrational modes in mediating energy transport among chlorophylls in the Light-harvesting Complex II (LHCII), the major light-harvesting complex in green plants. The vibrational modes are considered to be resonant/quasi-resonant with the energy gap between electronic excitons. These resonant vibrations, along with the remaining nuclear degrees of freedom, constitute the environment/bath to the electronically excited system and contribute to two major phenomena: (a) decoherence and (b) incoherent phonon-mediated population relaxation. In this work, we explore the subtle interplay among the electronic excitation, the resonant vibrations, and the environment in dictating environment assisted quantum transport in light-harvesting complexes. We conclusively show that resonant vibrations are capable of boosting the incoherent population relaxation pathways and cause rapid decoherence.

Topics & Concepts

Quantum decoherencePhysicsExcitonExcited stateRelaxation (psychology)ExcitationPopulationAtomic physicsVibrational energy relaxationPhononMolecular vibrationQuantumChemistryChemical physicsMolecular physicsQuantum mechanicsMoleculeDemographySocial psychologySociologyPsychologySpectroscopy and Quantum Chemical StudiesPhotosynthetic Processes and MechanismsElectrochemical Analysis and Applications
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