Enhancement of Vibronic and Ground-State Vibrational Coherences in 2D Spectra of Photosynthetic Complexes

被引:146
作者
Chenu, Aurelia [1 ]
Christensson, Niklas [2 ]
Kauffmann, Harald F. [2 ]
Mancal, Tomas [1 ]
机构
[1] Charles Univ Prague, Fac Math & Phys, CR-12116 Prague 2, Czech Republic
[2] Univ Vienna, Fac Phys, A-1090 Vienna, Austria
来源
SCIENTIFIC REPORTS | 2013年 / 3卷
基金
奥地利科学基金会;
关键词
2-DIMENSIONAL IR-SPECTROSCOPY; RESONANCE RAMAN-SPECTRA; ENERGY-TRANSFER; ELECTRONIC COHERENCE; QUANTUM COHERENCE; EXCITON DYNAMICS; REACTION CENTERS; BACTERIOCHLOROPHYLL; PROTEIN; EXCITATION;
D O I
10.1038/srep02029
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
A vibronic-exciton model is applied to investigate the recently proposed mechanism of enhancement of coherent oscillations due to mixing of electronic and nuclear degrees of freedom. We study a dimer system to elucidate the role of resonance coupling, site energies, vibrational frequency and energy disorder in the enhancement of vibronic-exciton and ground-state vibrational coherences, and to identify regimes where this enhancement is significant. For a heterodimer representing two coupled bachteriochloropylls of the FMO complex, long-lived vibronic coherences are found to be generated only when the frequency of the mode is in the vicinity of the electronic energy difference. Although the vibronic-exciton coherences exhibit a larger initial amplitude compared to the ground-state vibrational coherences, we conclude that, due to the dephasing of the former, both type of coherences have a similar magnitude at longer population time.
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页数:12
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