title: Energy-transfer and charge-separation pathways in the reaction center of photosystem II revealed by coherent two-dimensional optical spectroscopy.
abstract: The excited state dynamics and relaxation of electrons and holes in the photosynthetic reaction center of photosystem II are simulated using a two-band tight-binding model. The dissipative exciton and charge carrier motions are calculated using a transport theory, which includes a strong coupling to a harmonic bath with experimentally determined spectral density, and reduces to the Redfield, the Förster, and the Marcus expressions in the proper parameter regimes. The simulated third order two-dimensional signals, generated in the directions -k(1)+k(2)+k(3), k(1)-k(2)+k(3), and k(1)+k(2)-k(3), clearly reveal the exciton migration and the charge-separation processes.
authors.affiliation: Department of Chemistry, University of California, Irvine, Irvine, California 92697-2025, USA. darius.abramavicius@ff.vu.lt
authors.forename: Darius
authors.initials: D
authors.lastname: Abramavicius
authors.forename: Shaul
authors.initials: S
authors.lastname: Mukamel
mesh_terms: D004735:Energy Transfer; D008956:Models, Chemical; D015394:Molecular Structure; D055095:Optics and Photonics; D045332:Photosystem II Protein Complex / Q000737:chemistry*; D011789:Quantum Theory; D013057:Spectrum Analysis; D013816:Thermodynamics
chemical_list: D045332:Photosystem II Protein Complex