Efficient energy transfer in light-harvesting systems, I: optimal temperature, reorganization energy and spatial–temporal correlations

Authors:
  • JWJianlan Wu
    Jianlan Wu
  • FLFan Liu
    Fan Liu
  • YSYoung Shen
    Young Shen
  • JCJianshu Cao
    Jianshu Cao
  • RSRobert J Silbey
    Robert J Silbey
Open Access
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Abstract
Understanding the mechanisms of efficient and robust energy transfer in light-harvesting systems provides new insights for the optimal design of artificial systems. In this paper, we use the Fenna-Matthews-Olson (FMO) protein complex and phycocyanin 645 (PC 645) to explore the general dependence on physical parameters that help maximize the efficiency and maintain its stability. With the Haken-Strobl model, the maximal energy transfer efficiency (ETE) is achieved under an intermediate optimal value of dephasing rate. To avoid the infinite temperature assumption in the Haken-Strobl model and the failure of the Redfield equation in predicting the Forster rate behavior, we use the generalized Bloch-Redfield (GBR) equation approach to correctly describe dissipative exciton dynamics and find that maximal ETE can be achieved under various physical conditions, including temperature, reorganization energy, and spatial-temporal correlations in noise. We also identify regimes of reorganization energy where the ETE changes monotonically with temperature or spatial correlation and therefore cannot be optimized with respect to these two variables.

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