Origin of Long-Lived Coherences in Light-Harvesting Complexes

被引：349

作者：

Christensson, Niklas ^{[2
]}

Kauffmann, Harald F. ^{[2
,4
]}

Pullerits, Tonu ^{[3
]}

Mancal, Tomas ^{[1
]}

机构：

[1] Charles Univ Prague, Fac Math & Phys, CR-12116 Prague, Czech Republic

[2] Univ Vienna, Fac Phys, A-1090 Vienna, Austria

[3] Lund Univ, Dept Chem Phys, SE-22100 Lund, Sweden

[4] Vienna Univ Technol, Fac Phys, A-1040 Vienna, Austria

来源：

JOURNAL OF PHYSICAL CHEMISTRY B | 2012年 / 116卷 / 25期

基金：

瑞典研究理事会;

关键词：

MATTHEWS-OLSON COMPLEX; GREEN SULFUR BACTERIA; ANTENNA COMPLEXES; QUANTUM COHERENCE; ENERGY-TRANSFER; TEMPERATURE; DYNAMICS; BACTERIOCHLOROPHYLL; DIFFERENCE; ABSORPTION;

D O I：

10.1021/jp304649c

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：

A vibronic exciton model is applied to explain the long-lived oscillatory features in the two-dimensional (2D) electronic spectra of the Fenna-Matthews-Olson (FMO) complex. Using experimentally determined parameters and uncorrelated site energy fluctuations, the model predicts oscillations with dephasing times of 1.3 ps at 77 K, which is in a good agreement with the experimental results. These long-lived oscillations originate from the coherent superposition of vibronic exciton states with dominant contributions from vibrational excitations on the same pigment. The oscillations obtain a large amplitude due to excitonic intensity borrowing, which gives transitions with strong vibronic character a significant intensity despite the small Huang-Rhys factor. Purely electronic coherences are found to decay on a 200 fs time scale.

引用

页码：7449 / 7454

页数：6

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