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Multiscale photosynthetic and biomimetic excitation energy transfer

Nature Physics volume 8, pages 562–567 (2012)Cite this article

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Abstract

Recent evidence suggests that quantum coherence enhances excitation energy transfer (EET) through individual photosynthetic light-harvesting protein complexes (LHCs). Its role in vivo is unclear however, where transfer to chemical reaction centres (RCs) spans larger, multi-LHC/RC networks. Here we predict maximum coherence lengths possible in fully connected chromophore networks with the generic structural and energetic features of multi-LHC/RC networks. A renormalization analysis reveals the dependence of EET dynamics on multiscale, hierarchical network structure. Surprisingly, thermal decoherence rate declines at larger length scales for physiological parameters and coherence length is instead limited by localization due to static disorder. Physiological parameters support coherence lengths up to ∼ 5 nm, which is consistent with observations of solvated LHCs and invites experimental tests for intercomplex coherences in multi-LHC/RC networks. Results further suggest that a semiconductor quantum dot network engineered with hierarchically clustered structure and small static disorder may support coherent EET over larger length scales, at ambient temperatures.

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Figure 1: Structural hierarchy of the higher-plant light-harvesting machinery and renormalization flow of our analogous dimeric chromophore network hierarchy.
Figure 2: Multiscale tunnelling and decoherence rates in an ordered network (ε0(ij)=0), across the first seven hierarchy levels k (curves labelled by colour), as a function of network clustering C.
Figure 3: Scaling of dynamical crossover by thermal decoherence (XTk=Fk(2Δk(12))/(2Δk(12))) and localization by static disorder ().

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Acknowledgements

We are grateful to the following people for discussions and comments: B. Hankamer,M. Landsberg, E. Knauth, I. Ross, M. Sarovar, S. Hoyer, B. Whaley, A. Ishizaki, T. Calhoun, G. Schlau-Cohen, N. Ginsberg, J. Dawlaty, G. Fleming, P. Rebentrost,L. Vogt, A. Perdomo, M. Mohseni, A. Aspuru-Guzik, A. Olaya-Castro, S. Jang, R. Pfeifer,P. Rohde, E. Cavalcanti and R. McKenzie. A.K.R. thanks the Whaley and Fleming groups at UC Berkeley, and the Aspuru-Guzik group at Harvard, for hospitality. This work was supported by Australian Research Council grants CE110001013, FF0776191, DP1093287 and DP0986352 and a Dan David Prize doctoral scholarship.

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Authors and Affiliations

  1. Institute for Molecular Bioscience, University of Queensland, St Lucia, Queensland 4072, Australia

    A. K. Ringsmuth

  2. Centre for Engineered Quantum Systems, University of Queensland, St Lucia, Queensland 4072, Australia

    A. K. Ringsmuth, G. J. Milburn & T. M. Stace

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Contributions

A.K.R. suggested the multiscale, hierarchical approach of the study. T.M.S. proposed the renormalization analysis. A.K.R. and T.M.S. completed the calculations. A.K.R. wrote, and T.M.S. and G.J.M. edited, the manuscript. G.J.M. supervised the project and advised on calculations.

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Correspondence to A. K. Ringsmuth.

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Ringsmuth, A., Milburn, G. & Stace, T. Multiscale photosynthetic and biomimetic excitation energy transfer. Nature Phys 8, 562–567 (2012). https://doi.org/10.1038/nphys2332

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