Instantaneous Mapping of Coherently Coupled Electronic Transitions and Energy Transfers in a Photosynthetic Complex Using Angle-Resolved Coherent Optical Wave-Mixing

被引:78
作者
Mercer, Ian P. [1 ]
El-Taha, Yasin C. [2 ]
Kajumba, Nathaniel [2 ]
Marangos, Jonathan P. [2 ]
Tisch, John W. G. [2 ]
Gabrielsen, Mads [3 ]
Cogdell, Richard J. [3 ]
Springate, Emma [4 ]
Turcu, Edmund [4 ]
机构
[1] Univ Coll Dublin, Ctr Synth & Chem Biol, Sch Phys, Dublin 4, Ireland
[2] Univ London Imperial Coll Sci Technol & Med, Blackett Lab, Quantum Opt & Laser Sci Grp, London, England
[3] Univ Glasgow, Fac Biomed & Life Sci, Glasgow, Lanark, Scotland
[4] STFC Rutherford Appleton Lab, Cent Laser Facil, Didcot, Oxon, England
基金
英国生物技术与生命科学研究理事会; 英国工程与自然科学研究理事会;
关键词
AB-INITIO; SPECTROSCOPY; RELAXATION; ACIDOPHILA; GENERATION; DYNAMICS; PULSES; LH2; FS;
D O I
10.1103/PhysRevLett.102.057402
中图分类号
O4 [物理学];
学科分类号
0702 ;
摘要
Understanding the role of coherent electronic motion is expected to resolve general questions of importance in macromolecular energy transfer. We demonstrate a novel nonlinear optical method, angle-resolved coherent wave mixing, that separates out coherently coupled electronic transitions and energy transfers in an instantaneous two-dimensional mapping. Angular resolution of the signal is achieved by using millimeter laser beam waists at the sample and by signal relay to the far field; for this we use a high energy, ultrabroadband hollow fiber laser source. We reveal quantum electronic beating with a time-ordered selection of transition energies in a photosynthetic complex.
引用
收藏
页数:4
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