Long-Lived Electronic Coherence in Dissipative Exciton Dynamics of Light-Harvesting Complexes
By Christoph Kreisbeck, Tobias Kramer. 2012
227 citations recorded by the source corpus.
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 reali...
Subfields: Atomic and Molecular Physics, and Optics, Cellular and Molecular Neuroscience
View Paper: https://www.semanticscholar.org/paper/8685b8c83690f51068cd2e0885b4f711fb5a4d90
How researchers see this paper
The researchers whose trusted networks rank it highest, strongest advocate first. Every researcher gets a different order.
In Atomic and Molecular Physics, and Optics
In Cellular and Molecular Neuroscience
Citations in the corpus
- Delocalized excitons in natural light-harvesting complexes (2018, background): “HEOM calculations of absorption spectra (Hein et al., 2012) and 2DES echo spectra (Hein et al., 2012; Kreisbeck and Kramer, 2012) on the other hand provided support for coherence signal of electronic nature lasting up to about 500 fs, but in the absence of static disorder and other sources of…”