TY - JOUR
T1 - When vibrations interact
T2 - Ultrafast energy relaxation of vibrational pairs in polyatomic liquids
AU - Deàk, John C.
AU - Iwaki, Lawrence K.
AU - Dlott, Dana D.
N1 - Funding Information:
This work was supported by US Army Research Office contract DAAH04-96-1-0038 and Air Force Office of Scientific Research contract F49620-97-1-0056. Partial support is acknowledged from National Science Foundation DMR-9714843. LKI acknowledges support from an AASERT fellowship DAAHO4-95-1-0284.
PY - 1998/9/4
Y1 - 1998/9/4
N2 - The ultrafast IR-Raman technique is used to compare picosecond timescale vibrational energy relaxation (VR) of a polyatomic liquid, acetonitrile (CH3CN), following excitation of either a C-H stretching fundamental (~3000 cm-1) or a pair of vibrations at about the same energy, the CN stretch and C-C stretch. When the vibrational pair is excited via combination band pumping, the CN stretch lifetime decreases by more than an order of magnitude, and an oscillation is observed in the C-C stretch population. These studies of a pair of interacting vibrations on the same molecule provide insight into the complex behavior expected from vibrationally excited nascent products of chemical reactions of condensed-phase polyatomic molecules.
AB - The ultrafast IR-Raman technique is used to compare picosecond timescale vibrational energy relaxation (VR) of a polyatomic liquid, acetonitrile (CH3CN), following excitation of either a C-H stretching fundamental (~3000 cm-1) or a pair of vibrations at about the same energy, the CN stretch and C-C stretch. When the vibrational pair is excited via combination band pumping, the CN stretch lifetime decreases by more than an order of magnitude, and an oscillation is observed in the C-C stretch population. These studies of a pair of interacting vibrations on the same molecule provide insight into the complex behavior expected from vibrationally excited nascent products of chemical reactions of condensed-phase polyatomic molecules.
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U2 - 10.1016/S0009-2614(98)00814-8
DO - 10.1016/S0009-2614(98)00814-8
M3 - Article
AN - SCOPUS:0037750963
SN - 0009-2614
VL - 293
SP - 405
EP - 411
JO - Chemical Physics Letters
JF - Chemical Physics Letters
IS - 5-6
ER -