Long-Lived Electronic Coherence in Dissipative Exciton Dynamics of Light-Harvesting Complexes

Kreisbeck, Christoph and Kramer, Tobias (2012) Long-Lived Electronic Coherence in Dissipative Exciton Dynamics of Light-Harvesting Complexes. JOURNAL OF PHYSICAL CHEMISTRY LETTERS, 3 (19). pp. 2828-2833. ISSN 1948-7185,

Full text not available from this repository. (Request a copy)

Abstract

Recent experiments on light-harvesting complexes at ambient temperatures display oscillatory signals in two-dimensional spectroscopy. They suggest mechanisms supporting coherent exciton transport through molecular networks in noisy environments. We demonstrate a mechanism that relies on the continuum properties of the vibronic spectral density. We employ the spectral density of the Fenna-Matthews-Olson (FMO) complex and perform a nonperturbative calculation of two-dimensional spectra. They display long-lasting electronic coherence up to 0.3 Ps at a temperature of 277 K Two important properties of the spectral density found in the FMO complex emerge; (i) the coupling to higher-frequency vibrations is large, as required for efficient transport toward the reaction center, and (ii) the slope of the spectral density at zero frequency approaches zero. We demonstrate that electronic coherence and fast thermalization depend sensitively on the continuum part of the spectral density but can be simultaneously realized in molecular networks.

Item Type: Article
Uncontrolled Keywords: MATTHEWS-OLSON COMPLEX; GREEN SULFUR BACTERIA; QUANTUM COHERENCE; ENERGY-TRANSFER; PHYSIOLOGICAL TEMPERATURE; PHOTOSYNTHESIS; SPECTROSCOPY; EQUATIONS; EVOLUTION; COUPLINGS;
Subjects: 500 Science > 530 Physics
Divisions: Physics > Institute of Theroretical Physics > Alumni or Retired Professors > Group Tobias Kramer
Depositing User: Dr. Gernot Deinzer
Date Deposited: 05 May 2020 06:59
Last Modified: 05 May 2020 06:59
URI: https://pred.uni-regensburg.de/id/eprint/17956

Actions (login required)

View Item View Item