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Donatas Zigmantas. Portrait.

Donatas Zigmantas

Professor

Donatas Zigmantas. Portrait.

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

Author

  • James Lim
  • David Palecek
  • Felipe Caycedo-Soler
  • Craig N Lincoln
  • Javier Prior
  • Hans von Berlepsch
  • Susana F Huelga
  • Martin B Plenio
  • Donatas Zigmantas
  • Jürgen Hauer

Summary, in English

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.

Department/s

  • Chemical Physics
  • NanoLund: Centre for Nanoscience

Publishing year

2015

Language

English

Publication/Series

Nature Communications

Volume

6

Document type

Journal article

Publisher

Nature Publishing Group

Topic

  • Biophysics

Status

Published

ISBN/ISSN/Other

  • ISSN: 2041-1723