Multidimensional femtosecond correlation spectroscopies of electronic and vibrational excitations

被引:730
作者
Mukamel, S
机构
[1] Univ Rochester, Dept Chem, Rochester, NY 14627 USA
[2] Univ Rochester, Rochester Theory Ctr Opt Sci & Engn, Rochester, NY 14627 USA
关键词
coherent nonlinear spectroscopy; chromophore aggregates; protein dynamics; photosynthetic antennae; infrared echoes;
D O I
10.1146/annurev.physchem.51.1.691
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
Femtosecond visible and infrared analogues of multiple-pulse nuclear magnetic resonance techniques provide novel snapshot probes into the structure and electronic and vibrational dynamics of complex molecular assemblies such as photosynthetic antennae, proteins, and hydrogen-bonded liquids. A classical-oscillator description of these spectroscopies in terms of interacting quasiparticles (rather than transitions among global eigenstates) is developed and sets the stage for designing new pulse sequences and inverting the multidimensional signals to yield molecular structures. Considerable computational advantages and a clear physical insight into the origin of the response and the relevant coherence sizes are provided by a real-space analysis of the underlying coherence-transfer pathways in Liouville space.
引用
收藏
页码:691 / 729
页数:41
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