Anharmonic couplings underlying the ultrafast vibrational dynamics of hydrogen bonds in liquids |
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Authors: | Huse N Bruner B D Cowan M L Dreyer J Nibbering E T J Miller R J D Elsaesser T |
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Institution: | Max-Born-Institut für Nichtlineare Optik und Kurzzeitspektroskopie, 12489 Berlin, Germany. |
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Abstract: | 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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