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Tönu Pullerits. Portrait.

Tönu Pullerits

Professor

Tönu Pullerits. Portrait.

Origin of Long-Lived Coherences in Light-Harvesting Complexes

Author

  • Niklas Christensson
  • Harald F. Kauffmann
  • Tönu Pullerits
  • Tomas Mancal

Summary, in English

A vibronic exciton model is applied to explain the long-lived oscillatory features in the two-dimensional (2D) electronic spectra of the Fenna-Matthews-Olson (FMO) complex. Using experimentally determined parameters and uncorrelated site energy fluctuations, the model predicts oscillations with dephasing times of 1.3 ps at 77 K, which is in a good agreement with the experimental results. These long-lived oscillations originate from the coherent superposition of vibronic exciton states with dominant contributions from vibrational excitations on the same pigment. The oscillations obtain a large amplitude due to excitonic intensity borrowing, which gives transitions with strong vibronic character a significant intensity despite the small Huang-Rhys factor. Purely electronic coherences are found to decay on a 200 fs time scale.

Department/s

  • Chemical Physics
  • NanoLund: Centre for Nanoscience

Publishing year

2012

Language

English

Pages

7449-7454

Publication/Series

The Journal of Physical Chemistry Part B

Volume

116

Issue

25

Document type

Journal article

Publisher

The American Chemical Society (ACS)

Topic

  • Atom and Molecular Physics and Optics

Status

Published

ISBN/ISSN/Other

  • ISSN: 1520-5207