Real-Time Path Integral Simulation of Exciton-Vibration Dynamics in Light-Harvesting Bacteriochlorophyll Aggregates

Sohang Kundu, Nancy Makri

Research output: Contribution to journalArticlepeer-review

Abstract

The mechanism of excitation energy transfer in photoexcited bacteriochlorophyll (BChl) aggregates poses intriguing questions, which have important implications for the observed efficiency of photosynthesis. We investigate this process through fully quantum mechanical calculations of exciton-vibration dynamics in chains and rings of BChl a 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.

Original languageEnglish (US)
Pages (from-to)8783-8789
Number of pages7
JournalJournal of Physical Chemistry Letters
Volume11
Issue number20
DOIs
StatePublished - Oct 15 2020

ASJC Scopus subject areas

  • Materials Science(all)
  • Physical and Theoretical Chemistry

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