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CYCLOPROPYLACETYLENE STUDIED IN COLD FREE JET EXPANSION, ROOM TEMPERATURE GAS, AND DILUTE SOLUTION: TIER MODEL IVR

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Title: CYCLOPROPYLACETYLENE STUDIED IN COLD FREE JET EXPANSION, ROOM TEMPERATURE GAS, AND DILUTE SOLUTION: TIER MODEL IVR
Creators: Crum, Pam L.; Brown, Gordon G.; Douglass, Kevin O.; Johns, Brian C.; Dian, James E.; Nair, Pradeep M.; Yoo, Hyun S.; Pate, Brooks H.
Issue Date: 2005
Abstract: The vibrational dynamics of the first excited state of the acetylenic C-H stretch of cyclopropylacetylene (CPA) in both gas- and solution-phase are investigated. FTMW-detected infrared spectroscopy in a free jet expansion are used to investigate the dynamics of ultracold molecular-beam CPA, while ultrafast time-domain transient absorption spectroscopy is used to study the dynamics of CPA in gas and dilute solution at room-temperature. Good agreement among the results measured by different techniques was reported previously and improved time-domain results have recently provided excellent agreement as well as new dynamic information. Both FTMW-detected IR spectroscopy and femtosecond pump-probe spectroscopy show a very fast (\ { }0.6 ps) initial IVR rate of the first excited state of the acetylenic C-H stretch and oscillations on the timescales of 5 ps and 20 ps, which is evidence of partial population return into the first excited state of the C-H stretch of CPA. When CPA is solvated (0.05M CCl$_4$ solution), the IVR rate maintains the room-temperature isolated molecule value. The solvent contribution to the total relaxation rate in solution (k$_T$$_O$$_T$ = k$_I$$_V$$_R$ + k$_V$$_E$$_R$) is minor and the main effects of the solvent are attributed to pure dephasing effects that destroy the intramolecular coherence.
URI: http://hdl.handle.net/1811/30546
Other Identifiers: 2005-TD-02
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