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

Summary, in English

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.

• Author: Ben Brüggemann; Pär Kjellberg; Tönu Pullerits
• Department/s: Chemical Physics
• Publishing year: 2007
• Language: English
• Pages: 192-196
• Publication/Series: Chemical Physics Letters
• Volume: 444
• Issue: 1-3
• Links: http://dx.doi.org/10.1016/j.cplett.2007.07.002
• Document type: Journal article
• Publisher: Elsevier
• Topic: Atom and Molecular Physics and Optics
• Status: Published
• ISBN/ISSN/Other: ISSN: 0009-2614