Non-perturbative calculation of 2D spectra in heterogeneous systems: Exciton relaxation in the FMO complex

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Abstract

Experimental 2D frequency resolved spectra showing the relaxation of excitons in the photosynthetic antenna system FMO are reproduced by a multi-exciton density matrix approach explicitly including the external fields. The interference of the polarizations of a number of randomly placed, rotated and energetically inhomogencous complexes is used to extract the signal in the phase matching directions. It is shown that varying the laser intensity has only a minor impact, but changing the phase within the single pulses makes higher order contributions possible which lead to a fundamental change of the 2D spectra. (C) 2007 Elsevier B.V. All rights reserved.

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  • Atom and Molecular Physics and Optics
Original languageEnglish
Pages (from-to)192-196
JournalChemical Physics Letters
Volume444
Issue number1-3
Publication statusPublished - 2007
Publication categoryResearch
Peer-reviewedYes

Bibliographic note

The information about affiliations in this record was updated in December 2015. The record was previously connected to the following departments: Chemical Physics (S) (011001060)