Real-Time Path Integral Simulation of Exciton-Vibration Dynamics in Light-Harvesting Bacteriochlorophyll Aggregates
Sohang Kundu, Nancy Makri
Abstract
molecules, with parameters characterizing the B850 ring of the LH2 complex of photosynthetic bacteria. The calculations are performed using the modular path integral methodology, which allows the exact treatment of 50 intramolecular vibrations on each pigment using parameters obtained from spectroscopic Huang-Rhys factors with computational effort that scales linearly with aggregate length. Our results indicate that the interplay between electronic and vibrational time scales leads to the rapid suppression but not the overdamping of electronic coherence, which facilitates the spreading of excitation energy throughout the aggregate.
Topics & Concepts
ChlorosomeExcitonBacteriochlorophyllIntramolecular forceExcitationCoherence (philosophical gambling strategy)Chemical physicsPath integral formulationVibrationPurple bacteriaQuantumPhysicsMolecular physicsChemistryMaterials sciencePhotosynthesisQuantum mechanicsPhotosynthetic reaction centreBiochemistrySpectroscopy and Quantum Chemical StudiesPhotosynthetic Processes and MechanismsAtmospheric Ozone and Climate