The flow of energy in light harvesting aggregates poses intriguing questions and has been the subject of intense theoretical and experimental work.  Because of the large size of these systems, previous simulations have included only a few vibrational degrees of freedom or have utilized simplified system-bath models.  We have used the modular path integral (MPI) methodology to present all-mode, fully quantum mechanical simulations of exciton-vibration dynamics in linear or ring-shaped bacteriochlorophyll complexes, which contain up to 16 molecular units, each with the two relevant electronic states and 50 normal mode vibrations whose parameters are obtained from spectroscopically determined Huang-Rhys factors, over a range of temperatures.  The MPI methodology proceeds by sequential linking of the quantum paths representing adjacent modules, which may include any number of molecular (or phonon) vibrations, and requires computational effort that scales linearly with the number of units, circumventing the exponential scaling of wavefunction-based quantum mechanical methods.  The simulations shed light on the intricate interplay among electronic coherence, linear vs. circular topology, Hilbert space size, and decoherence induced by chlorophyll vibrations and thermal fluctuations.<br/> <br/>

Modular path integral simulation of exciton-vibration dynamics in large light harvesting complexes

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.