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Instantaneous Mapping of Coherently Coupled Electronic Transitions and Energy Transfers in a Photosynthetic Complex Using Angle-Resolved Coherent Optical Wave-Mixing

Ian P. Mercer, Yasin C. El-Taha, Nathaniel Kajumba, Jonathan P. Marangos, John W. G. Tisch, Mads Gabrielsen, Richard J. Cogdell, Emma Springate, and Edmund Turcu
Phys. Rev. Lett. 102, 057402 – Published 6 February 2009
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Abstract

Understanding the role of coherent electronic motion is expected to resolve general questions of importance in macromolecular energy transfer. We demonstrate a novel nonlinear optical method, angle-resolved coherent wave mixing, that separates out coherently coupled electronic transitions and energy transfers in an instantaneous two-dimensional mapping. Angular resolution of the signal is achieved by using millimeter laser beam waists at the sample and by signal relay to the far field; for this we use a high energy, ultrabroadband hollow fiber laser source. We reveal quantum electronic beating with a time-ordered selection of transition energies in a photosynthetic complex.

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  • Received 19 September 2008

DOI:https://doi.org/10.1103/PhysRevLett.102.057402

©2009 American Physical Society

Authors & Affiliations

Ian P. Mercer1, Yasin C. El-Taha2, Nathaniel Kajumba2, Jonathan P. Marangos2, John W. G. Tisch2, Mads Gabrielsen3, Richard J. Cogdell3, Emma Springate4, and Edmund Turcu4

  • 1School of Physics, Centre for Synthesis and Chemical Biology, University College Dublin, Dublin 4, Ireland
  • 2Quantum Optics and Laser Science Group, Blackett Laboratory, Imperial College, London, United Kingdom
  • 3Biochemistry and Molecular Biology, Faculty of Biomedical and Life Sciences, University of Glasgow, Glasgow, United Kingdom
  • 4Central Laser Facility, STFC Rutherford Appleton Laboratory, Didcot, United Kingdom

See Also

The Quantum Dimension Of Photosynthesis

Michael Schirber
Phys. Rev. Focus 23, 5 (2009)

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Vol. 102, Iss. 5 — 6 February 2009

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