A stochastic surrogate Hamiltonian approach of coherent and incoherent exciton transport in the Fenna-Matthews-Olson complex

Abstract

The capture and transduction of energy in biological systems is clearly necessary for life, and nature has evolved remarkable macromolecular entities to serve these purposes. The Fenna-Matthews-Olson (FMO) complex serves as an intermediate to transfer the energy from the chlorosome to the special pairs of different photo systems. Recent observations have both suggested the importance of coherent exciton transport within the FMO and motivated an elegant and appropriate theoretical construct for interpreting these observations. Here we employ a different approach to exciton transport in a relaxing environment, one based on the stochastic surrogate Hamiltonian method. With it, we calculate the quantum trajectories through the FMO complex both for the model involving seven bacteriochlorophylls that has been used before, and for one involving an eighth bacteriochlorophyll, which has been observed in some new and very important structural work. We find that in both systems, efficient energy transfer to the ultimate receptor occurs, but that because of the placement of, and energy relaxation among, the different bacteriochlorophyll subunits in the FMO complex, the importance of coherent oscillation that was discussed extensively for the seven site system is far less striking for the eight site system, effectively because of the weak mixing between the initial site and the remainder of the system. We suggest that the relevant spectral densities can be determinative for the energy transport route and may provide a new way to enhance energy transfer in artificial devices.

Document Details

Document Type
Pub Defense Publication
Publication Date
Aug 17, 2011
Source ID
10.1063/1.3624376

Entities

People

  • M. A. Ratner
  • N. Renaud
  • V. Mujica

Organizations

  • Argonne National Laboratory
  • Arizona State University
  • Defense Advanced Research Projects Agency
  • Northwestern University
  • United States Department of Energy

Tags

Readers

  • Quantum Chemistry
  • Quantum Dot Semiconductor Device Photonics and Graphene Optoelectronic Materials and THz Physics.
  • Systems Analysis and Design

Technology Areas

  • Microelectronics
  • Quantum Computing