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Vibronic origin of long-lived coherence in an artificial molecular light harvester

Author

Listed:
  • James Lim

    (Institut für Theoretische Physik, Universität Ulm)

  • David Paleček

    (Lund University
    Charles University in Prague)

  • Felipe Caycedo-Soler

    (Institut für Theoretische Physik, Universität Ulm)

  • Craig N. Lincoln

    (Photonics Institute, Vienna University of Technology)

  • Javier Prior

    (Universidad Politécnica de Cartagena)

  • Hans von Berlepsch

    (Forschungszentrum für Elektronenmikroskopie, Institut für Chemie und Biochemie, Freie Universität Berlin)

  • Susana F. Huelga

    (Institut für Theoretische Physik, Universität Ulm)

  • Martin B. Plenio

    (Institut für Theoretische Physik, Universität Ulm)

  • Donatas Zigmantas

    (Lund University)

  • Jürgen Hauer

    (Photonics Institute, Vienna University of Technology)

Abstract

Natural and artificial light-harvesting processes have recently gained new interest. Signatures of long-lasting coherence in spectroscopic signals of biological systems have been repeatedly observed, albeit their origin is a matter of ongoing debate, as it is unclear how the loss of coherence due to interaction with the noisy environments in such systems is averted. Here we report experimental and theoretical verification of coherent exciton–vibrational (vibronic) coupling as the origin of long-lasting coherence in an artificial light harvester, a molecular J-aggregate. In this macroscopically aligned tubular system, polarization-controlled 2D spectroscopy delivers an uncongested and specific optical response as an ideal foundation for an in-depth theoretical description. We derive analytical expressions that show under which general conditions vibronic coupling leads to prolonged excited-state coherence.

Suggested Citation

  • James Lim & David Paleček & Felipe Caycedo-Soler & Craig N. Lincoln & Javier Prior & Hans von Berlepsch & Susana F. Huelga & Martin B. Plenio & Donatas Zigmantas & Jürgen Hauer, 2015. "Vibronic origin of long-lived coherence in an artificial molecular light harvester," Nature Communications, Nature, vol. 6(1), pages 1-7, November.
    • Handle: RePEc:nat:natcom:v:6:y:2015:i:1:d:10.1038_ncomms8755
    DOI: 10.1038/ncomms8755
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