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APPLICATIONS OF A SINGLE-PULSE BROADBAND FTMW SPECTROMETER: THE DYANMIC ROTATIONAL SPECTRUM OF 4-FLUOROBUT-1-YNE

Please use this identifier to cite or link to this item: http://hdl.handle.net/1811/30617

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Title: APPLICATIONS OF A SINGLE-PULSE BROADBAND FTMW SPECTROMETER: THE DYANMIC ROTATIONAL SPECTRUM OF 4-FLUOROBUT-1-YNE
Creators: Dian, Brian C.; Douglass, Kevin O.; Brown, Gordon G.; Geyer, Scott M.; Pate, Brooks H.
Issue Date: 2005
Abstract: We perform dynamic rotational spectroscopy on vibrationally excited 4-fluorobut-1-yne using our state-of-the-art, chirped-pulse broadband spectrometer. This new spectrometer allowed us to record 11 GHz of spectrum (7.5-18 GHz) with a single microwave pulse to study the energy-dependence of the isomerization kinetics, dramatically reducing data acquisition times. 4-Fluorobut-1-yne is an asymmetric top found in one of two conformers in a supersonic expansion, with fluorine either {\it trans} or {\it gauche} with respect to the ethynyl group. The {\it trans- gauche} isomerization barrier is approximately 1377 $\wn$, and the {\it trans} form is more stable by 492 $\wn$. Infrared laser excitation was used to prepare 4-fluorobut-1-yne in a region of the potential surface where isomerization can occur ( 3000 $\wn$). Using our broadband spectrometer, the rotational spectrum of the infrared excited molecule was recorded from 7.5-18 GHz, covering the $\Delta$J = 1$\rightarrow$2 and $\Delta$J = 2$\rightarrow$3 regions of the spectrum. The overall lineshape of the rotational spectrum was fit with a three-state Bloch model, modified for chemical exchange, yielding an isomerization rate of k$_iso$ = 2.7x10$^{10}$ s$^{-1}$, much slower than the rate predicted by RRKM theory: k$_iso$ = 5.9x10$^{11}$ s$^{-1}$. The single eigenstate rotational spectra recorded with our newly developed spectrometer agree with previously measured single eigenstate rotational spectra, recorded in the acetylenic CH-stretch at 3330 $\wn$. Using a combination of double (infrared-microwave) and triple resonance (infrared-microwave-microwave) techniques, single eigenstate rotational spectra were recorded for several IR bands. Infrared excitation of the various CH-stretching bands allows us to observe the isomerization dynamics over a broad energy range (2900-3330 $\wn$). Observed changes on the rotational spectrum will be discussed.
URI: http://hdl.handle.net/1811/30617
Other Identifiers: 2005-TI-10
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