Strongly coupled bacteriochlorin dyad studied using phase-modulated fluorescence-detected two-dimensional electronic spectroscopy

被引:39
作者
Tiwari, Vivek [1 ]
Matutes, Yassel Acosta [2 ]
Konar, Arkaprabha [1 ]
Yu, Zhanqian [3 ]
Ptaszek, Marcin [3 ]
Bocian, David F. [4 ]
Holten, Dewey [5 ]
Kirmaier, Christine [5 ]
Ogilvie, Jennifer P. [1 ]
机构
[1] Univ Michigan, Dept Phys, Ann Arbor, MI 48109 USA
[2] Univ Michigan, Appl Phys Program, Ann Arbor, MI 48109 USA
[3] Univ Maryland Baltimore Cty, Dept Chem & Biochem, Baltimore, MD 21250 USA
[4] Univ Calif Riverside, Dept Chem, Riverside, CA 92521 USA
[5] Washington Univ, Dept Chem, St Louis, MO 63130 USA
基金
美国国家科学基金会;
关键词
RESONANCE RAMAN-SPECTRA; ENERGY-TRANSFER; VIBRONIC COHERENCE; VIBRATIONAL-MODES; QUANTUM COHERENCE; REACTION CENTERS; LIGHT; COMPLEXES; DYNAMICS; SYSTEMS;
D O I
10.1364/OE.26.022327
中图分类号
O43 [光学];
学科分类号
070207 ; 0803 ;
摘要
Fluorescence-detected two-dimensional electronic spectroscopy (F-2DES) projects the third-order non-linear polarization in a system as an excited electronic state population which is incoherently detected as fluorescence. Multiple variants of F-2DES have been developed. Here, we report phase-modulated F-2DES measurements on a strongly coupled symmetric bacteriochlorin dyad. a relevant 'toy' model for photosynthetic energy and charge transfer. Coherence map analysis shows that the strongest frequency observed in the dyad is well-separated from the excited state electronic energy gap, and is consistent with a vibrational frequency readily observed in bacteriochlorin monomers. Kinetic rate maps show a picosecond relaxation timescale between the excited states of the dyad. To our knowledge this is the first demonstration of coherence and kinetic analysis using the phase-modulation approach to F-2DES. (C) 2018 Optical Society of America under the terms of the OSA Open Access Publishing Agreement
引用
收藏
页码:22327 / 22341
页数:15
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