Infrared laser spectroscopy of CH3...HF in helium nanodroplets: The exit-channel complex of the F + CH4 reaction

The Journal of Chemical Physics
Jeremy M MerrittRoger E Miller

Abstract

High-resolution infrared laser spectroscopy is used to study the CH3...HF and CD3...HF radical complexes, corresponding to the exit-channel complex in the F + CH4 --> HF + CH3 reaction. The complexes are formed in helium nanodroplets by sequential pickup of a methyl radical and a HF molecule. The rotationally resolved spectra presented here correspond to the fundamental v = 1 <-- 0 H-F vibrational band, the analysis of which reveals a complex with C(3v) symmetry. The vibrational band origin for the CH3...HF complex (3797.00 cm(-1)) is significantly redshifted from that of the HF monomer (3959.19 cm(-1)), consistent with the hydrogen-bonded structure predicted by theory [E. Ya. Misochko et al., J. Am. Chem. Soc. 117, 11997 (1995)] and suggested by previous matrix isolation experiments [M. E. Jacox, Chem. Phys. 42, 133 (1979)]. The permanent electric dipole moment of this complex is experimentally determined by Stark spectroscopy to be 2.4+/-0.3 D. The wide amplitude zero-point bending motion of this complex is revealed by the vibrational dependence of the A rotational constant. A sixfold reduction in the line broadening associated with the H-F vibrational mode is observed in going from CH3...HF to CD3...HF. The results suggest t...Continue Reading

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Citations

Mar 5, 2009·The Journal of Chemical Physics·Gábor CzakóJoel M Bowman
Jul 26, 2006·The Journal of Chemical Physics·Aleksandra A MikoszDavid Farrelly
Sep 22, 2011·The Journal of Chemical Physics·J FedorM Fárník
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Aug 3, 2014·The Journal of Chemical Physics·Daniel HabigMartina Havenith
Jan 20, 2015·The Journal of Physical Chemistry. a·Daniel LeichtMartina Havenith
Jun 6, 2009·Journal of the American Chemical Society·Steen Hammerum
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Jun 25, 2009·Physical Chemistry Chemical Physics : PCCP·Svemir RudićRoger E Miller
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May 9, 2014·Physical Chemistry Chemical Physics : PCCP·Qingzhong LiHai-Bei Li
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