Modelling of oscillations in two-dimensional echo-spectra of the Fenna–Matthews–Olson complex

By Birgit Hein, Christoph Kreisbeck, Tobias Kramer, Mirta Rodr'iguez. 2011

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Recent experimental observations of time-dependent beatings in the two-dimensional echo-spectra of light-harvesting complexes at ambient temperatures have opened up the question of whether coherence and wave-like behaviour play a significant role in photosynthesis. We carry out a numerical study of the absorption and echo-spectra of the Fenna–Matthews–Olson (FMO) complex in Chlorobium tepidum and analyse the requirements in the theoretical model needed to reproduce beatings in the calculated spectra. The energy transfer in the FMO pigment–protein complex is theoretically described by an exciton Hamiltonian coupled to a phonon bath which accounts for the pigments' electronic and vibrational excitations, respectively. We use the hierarchical equations of motions method to treat the strong couplings in a non-perturbative way. We show that the oscillations in the two-dimensional echo-spectra persist in the presence of thermal noise and static disorder.

Subfields: Atomic and Molecular Physics, and Optics, Molecular Biology

View Paper: https://www.semanticscholar.org/paper/bdca9d410dbd99cc4a5d27d060d3b3f92558bcd7

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In Atomic and Molecular Physics, and Optics

In Molecular Biology

Citations in the corpus

Vibrations, quanta and biology (2013, methodology): “calculations of 2-D spectra [161] using this method and recent algorithmic improvements [162].”
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…”