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

被引：57

作者：

Bruggemann, Ben ^{[1
]}

Kjellberg, Par ^{[1
]}

Pullerits, Tonu ^{[1
]}

机构：

[1] Lund Univ, Dept Chem Phys, S-22100 Lund, Sweden

来源：

CHEMICAL PHYSICS LETTERS | 2007年 / 444卷 / 1-3期

关键词：

D O I：

10.1016/j.cplett.2007.07.002

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

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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收藏

页码：192 / 196

页数：5

相关论文

共 35 条

[1] Hydrogen bond dynamics probed with ultrafast infrared heterodyne-detected multidimensional vibrational stimulated echoes [J].

Asbury, JB ;

Steinel, T ;

Stromberg, C ;

Gaffney, KJ ;

Piletic, IR ;

Goun, A ;

Fayer, MD .

PHYSICAL REVIEW LETTERS, 2003, 91 (23)

[2] Two-dimensional infrared spectroscopy of peptides by phase-controlled femtosecond vibrational photon echoes [J].

Asplund, MC ;

Zanni, MT ;

Hochstrasser, RM .

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2000, 97 (15) :8219-8224

[3] PROPERTIES OF THE EXCITED-SINGLET STATES OF BACTERIOCHLOROPHYLL-A AND BACTERIOPHEOPHYTIN-A IN POLAR-SOLVENTS [J].

BECKER, M ;

NAGARAJAN, V ;

PARSON, WW .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1991, 113 (18) :6840-6848

[4] Two-dimensional spectroscopy of electronic couplings in photosynthesis [J].

Brixner, T ;

Stenger, J ;

Vaswani, HM ;

Cho, M ;

Blankenship, RE ;

Fleming, GR .

NATURE, 2005, 434 (7033) :625-628

[5] Phase-stabilized two-dimensional electronic spectroscopy [J].

Brixner, T ;

Mancal, T ;

Stiopkin, IV ;

Fleming, GR .

JOURNAL OF CHEMICAL PHYSICS, 2004, 121 (09) :4221-4236

[6] Controlling excitonic wavepacket motion in the PS1 core-antenna system [J].

Brüggemann, B ;

May, V .

CHEMICAL PHYSICS LETTERS, 2004, 400 (4-6) :573-577

[7] Ultrafast laser pulse control of exciton dynamics:: A computational study on the FMO complex [J].

Brüggemann, B ;

May, V .

JOURNAL OF PHYSICAL CHEMISTRY B, 2004, 108 (29) :10529-10539

[8] Exciton exciton annihilation dynamics in chromophore complexes.: II.: Intensity dependent transient absorption of the LH2 antenna system [J].

Brüggemann, B ;

May, V .

JOURNAL OF CHEMICAL PHYSICS, 2004, 120 (05) :2325-2336

[9] Exciton exciton annihilation dynamics in chromophore complexes.: I.: Multiexciton density matrix formulation [J].

Brüggemann, B ;

May, V .

JOURNAL OF CHEMICAL PHYSICS, 2003, 118 (02) :746-759

[10] Laser pulse control of exciton dynamics in the FMO complex:: Polarization shaping versus effects of structural and energetic disorder [J].

Bruggemann, Ben ;

Pullerits, Tonu ;

May, Volkhard .

JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY, 2006, 180 (03) :322-327

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