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The role of non-equilibrium vibrational structures in electronic coherence and recoherence in pigment–protein complexes

Nature Physics volume 9, pages 113–118 (2013)Cite this article

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Abstract

Recent observations of oscillatory features in the optical response of photosynthetic complexes have revealed evidence for surprisingly long-lasting electronic coherences which can coexist with energy transport. These observations have ignited multidisciplinary interest in the role of quantum effects in biological systems, including the fundamental question of how electronic coherence can survive in biological surroundings. Here we show that the non-trivial spectral structures of protein fluctuations can generate non-equilibrium processes that lead to the spontaneous creation and sustenance of electronic coherence, even at physiological temperatures. Developing new advanced simulation tools to treat these effects, we provide a firm microscopic basis to successfully reproduce the experimentally observed coherence times in the Fenna–Matthews–Olson complex, and illustrate how detailed quantum modelling and simulation can shed further light on a wide range of other non-equilibrium processes which may be important in different photosynthetic systems.

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Figure 1: The generic organization of the early stages of light-harvesting in natural photosynthesis.
Figure 2: Electronic coherence from the semiclassical model.
Figure 3: Numerical exact results of electronic coherence for cryogenic and physiological temperatures.
Figure 4: Spontaneous generation of excitonic coherence.

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Acknowledgements

This work was supported by the Alexander von Humboldt-Foundation, the EU STREP project PICC and the EU Integrated Project Q-ESSENCE. A.W.C. acknowledges support from the Winton Programme for the Physics of Sustainability. J.P. was supported by Ministerio de Ciencia e Innovación Project No. FIS2009-13483-C02-02 and the Fundación Séneca Project No. 11920/PI/09-j. We acknowledge the bwGRiD project (http://www.bw-grid.de) for the computational resources. Aspects of this work have benefited from discussions with J. Almeida, A. G. Dijkstra, D. Hayes, J. Caram, G. S. Engel and R. van Grondelle.

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Authors and Affiliations

  1. Institute of Theoretical Physics, Universität Ulm, Albert-Einstein-Allee 11, 89069 Ulm, Germany

    A. W. Chin, R. Rosenbach, F. Caycedo-Soler, S. F. Huelga & M. B. Plenio

  2. Theory of Condensed Matter Group, Cavendish Laboratory, University of Cambridge, J J Thomson Avenue, Cambridge, CB3 0HE, UK

    A. W. Chin

  3. Departamento de Física Aplicada, Universidad Politécnica de Cartagena, Cartagena 30202, Spain

    J. Prior

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Contributions

S.F.H. and M.B.P. designed the research with input from A.W.C.; A.W.C. and F.C-S. carried out the analytical calculations with advice from S.F.H. and M.B.P.; J.P. and R.R. developed the numerical codes and carried out the numerical simulations with guidance from A.W.C. and M.B.P. All authors discussed the results. S.F.H. and M.B.P. led the project. A.W.C., F.C.S., S.F.H. and M.B.P. wrote the manuscript with input of all authors.

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Correspondence to M. B. Plenio.

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Chin, A., Prior, J., Rosenbach, R. et al. The role of non-equilibrium vibrational structures in electronic coherence and recoherence in pigment–protein complexes. Nature Phys 9, 113–118 (2013). https://doi.org/10.1038/nphys2515

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