Origin of Long-Lived Coherences in Light-Harvesting Complexes

Niklas Christensson; Harald Kauffmann; Tönu Pullerits; Tomas Mancal

doi:10.1021/jp304649c

Origin of Long-Lived Coherences in Light-Harvesting Complexes

Niklas Christensson, Harald Kauffmann, Tönu Pullerits, Tomas Mancal (Corresponding author)

Electronic Properties of Materials

Publications: Contribution to journal › Article › Peer Reviewed

Abstract

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.

Original language	English
Pages (from-to)	7449-7454
Number of pages	6
Journal	The Journal of Physical Chemistry Part B: Condensed Matter, Materials, Surfaces, Interfaces & Biophysical
Volume	116
Issue number	25
DOIs	https://doi.org/10.1021/jp304649c
Publication status	Published - 2012

Austrian Fields of Science 2012

104017 Physical chemistry
1030 Physics, Astronomy

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10.1021/jp304649c

http://arxiv.org/abs/1201.6325

Cite this

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abstract = "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.",

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AU - Christensson, Niklas

AU - Kauffmann, Harald

AU - Pullerits, Tönu

AU - Mancal, Tomas

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N2 - 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.

AB - 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.

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JF - The Journal of Physical Chemistry Part B: Condensed Matter, Materials, Surfaces, Interfaces & Biophysical

IS - 25

ER -

Origin of Long-Lived Coherences in Light-Harvesting Complexes

Abstract

Austrian Fields of Science 2012

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