Anharmonic couplings underlying the ultrafast vibrational dynamics of hydrogen bonds in liquids

被引:74
作者
Huse, N [1 ]
Bruner, BD
Cowan, ML
Dreyer, J
Nibbering, ETJ
Miller, RJD
Elsaesser, T
机构
[1] Max Born Inst Nichtlineare & Kurzzeitspektroskopi, D-12489 Berlin, Germany
[2] Univ Toronto, Dept Phys, Toronto, ON M5S 3H6, Canada
[3] Univ Toronto, Dept Chem, Toronto, ON M5S 3H6, Canada
关键词
D O I
10.1103/PhysRevLett.95.147402
中图分类号
O4 [物理学];
学科分类号
0702 ;
摘要
The multilevel structure and vibrational couplings of O - H stretching transitions in intermolecular hydrogen bonds of acetic acid dimers are determined by femtosecond two-dimensional photon-echo spectroscopy in the infrared. Combining experiment and theoretical calculations, we separate Fermi resonances with combination tones of fingerprint modes from anharmonic couplings to underdamped low-frequency modes of the dimer. A multilevel density matrix approach based on density functional theory calculations reproduces the experimental results and reveals coupling strengths of both mechanisms on the order of 40-150 cm(-1).
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页数:4
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