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

Ben Brüggemann; Pär Kjellberg; Tönu Pullerits

doi:10.1016/j.cplett.2007.07.002

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

Ben Brüggemann, Pär Kjellberg, Tönu Pullerits

Chemical Physics

Research output: Contribution to journal › Article › peer-review

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.

Original language	English
Pages (from-to)	192-196
Journal	Chemical Physics Letters
Volume	444
Issue number	1-3
DOIs	https://doi.org/10.1016/j.cplett.2007.07.002
Publication status	Published - 2007

Bibliographical 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)

Subject classification (UKÄ)

Atom and Molecular Physics and Optics

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10.1016/j.cplett.2007.07.002

Cite this

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

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.",

author = "Ben Br{\"u}ggemann and P{\"a}r Kjellberg and T{\"o}nu Pullerits",

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)",

year = "2007",

doi = "10.1016/j.cplett.2007.07.002",

language = "English",

volume = "444",

pages = "192--196",

journal = "Chemical Physics Letters",

issn = "0009-2614",

publisher = "Elsevier",

number = "1-3",

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T1 - Non-perturbative calculation of 2D spectra in heterogeneous systems: Exciton relaxation in the FMO complex

AU - Brüggemann, Ben

AU - Kjellberg, Pär

AU - Pullerits, Tönu

N1 - 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)

PY - 2007

Y1 - 2007

N2 - 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.

AB - 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.

U2 - 10.1016/j.cplett.2007.07.002

DO - 10.1016/j.cplett.2007.07.002

M3 - Article

SN - 0009-2614

VL - 444

SP - 192

EP - 196

JO - Chemical Physics Letters

JF - Chemical Physics Letters

IS - 1-3

ER -

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

Abstract

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