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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共 19 条
[11]   Ultrafast relaxation and anharmonic coupling of O-H stretching and bending excitations in cyclic acetic acid dimers [J].
Heyne, K ;
Huse, N ;
Nibbering, ETJ ;
Elsaesser, T .
CHEMICAL PHYSICS LETTERS, 2003, 382 (1-2) :19-25
[12]   Vibrational multilevel quantum coherence due to anharmonic couplings in intermolecular hydrogen bonds [J].
Huse, N ;
Heyne, K ;
Dreyer, J ;
Nibbering, ETJ ;
Elsaesser, T .
PHYSICAL REVIEW LETTERS, 2003, 91 (19) :197401/1-197401/4
[13]   Two-dimensional femtosecond spectroscopy [J].
Jonas, DM .
ANNUAL REVIEW OF PHYSICAL CHEMISTRY, 2003, 54 :425-463
[14]   Linear techniques of phase measurement by femtosecond spectral interferometry for applications in spectroscopy [J].
Lepetit, L ;
Cheriaux, G ;
Joffre, M .
JOURNAL OF THE OPTICAL SOCIETY OF AMERICA B-OPTICAL PHYSICS, 1995, 12 (12) :2467-2474
[15]   Unusual vibrational dynamics of the acetic acid dimer [J].
Lim, M ;
Hochstrasser, RM .
JOURNAL OF CHEMICAL PHYSICS, 2001, 115 (16) :7629-7643
[16]   INFRARED SPECTRA OF H-BONDED SYSTEMS [J].
MARECHAL, Y ;
WITKOWSKI, A .
JOURNAL OF CHEMICAL PHYSICS, 1968, 48 (08) :3697-+
[17]   Multidimensional femtosecond correlation spectroscopies of electronic and vibrational excitations [J].
Mukamel, S .
ANNUAL REVIEW OF PHYSICAL CHEMISTRY, 2000, 51 :691-729
[18]  
Mukamel S., 1999, PRINCIPLES NONLINEAR
[19]   Ultrafast vibrational dynamics of hydrogen bonds in the condensed phase [J].
Nibbering, ETJ ;
Elsaesser, T .
CHEMICAL REVIEWS, 2004, 104 (04) :1887-1914