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Effects of C–H stretch excitation on the reaction
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10.1063/1.2034507
/content/aip/journal/jcp/123/13/10.1063/1.2034507
http://aip.metastore.ingenta.com/content/aip/journal/jcp/123/13/10.1063/1.2034507
View: Figures

Figures

Image of FIG. 1.
FIG. 1.

Energetics for the reaction. The total energy available for the reaction is given by the sum of the translational and vibrational energies, and the five different combinations probed in this work are described by Eqs. (2a)–(2e) in the text. The collision energy broadening is calculated by the formulas of van der Zande et al. (Ref. 68). Selected and product-state energy levels are given on the right side.

Image of FIG. 2.
FIG. 2.

Action spectrum recorded while monitoring the stretch-excited from the reaction at while the IR laser is scanned over the absorption feature indicating that the observed enhancement arises from methane vibration. The line positions of the , , and branches are obtained from the HITRAN database (Ref. 69).

Image of FIG. 3.
FIG. 3.

Product REMPI spectra for the reactions: (a) , (b) , and (c) for a center-of-mass collision energy . From the left the positions of the (C–H stretch overtone), (C–H stretch), (ground state), (symmetric stretching and umbrella bending combination), and (umbrella bending mode) bands are marked by the vertical dotted lines. The signal when the IR laser is off is the ground-state signal and (b) is the difference obtained while the IR laser pumps the branch while (c) is the difference obtained while the IR laser pumps the branch.

Image of FIG. 4.
FIG. 4.

Product REMPI spectra for the reactions: (a) and (b) for a center-of-mass collision energy . Reading from left to right, the positions of the (C–H stretch), (ground state), (symmetric stretching and umbrella bending combination), and (umbrella bending mode) bands are marked by the vertical dotted lines. The signal when the IR laser is off is the ground-state signal and (b) is the difference obtained while the IR laser pumps the branch. Within the experimental uncertainty no difference is observed between the spectra recorded at and those obtained at (Fig. 3).

Image of FIG. 5.
FIG. 5.

Relative enhancement, , for the reaction channel as a function of the center-of-mass collision energy . The constant is chosen such that the enhancement factor for . The uncertainty given is the statistical 95% confidence interval from replicate measurements.

Image of FIG. 6.
FIG. 6.

Isotropic (엯) and anisotropic (◻) TOF profiles (left panel) and laboratory-frame speed distributions (right panel) of the state-to-state selected products for (a) observed on the band branch, (b) , and (c) observed on the band branch. The uncertainty given is one standard deviation of replicate measurements and within this uncertainty the measured distributions are the indistinguishable.

Image of FIG. 7.
FIG. 7.

Product REMPI spectra for the reactions: (a) , (b) , and (c) at a center-of-mass collision energy of . Reading from left to right, the positions of the (C–H stretch), (ground state), and (umbrella bending mode) bands are marked by the vertical dotted lines. (a) displays the signal when the IR laser is off ; (b) displays the difference obtained while the IR laser pumps the branch; and (c) displays the difference obtained while the IR laser pumps the branch.

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/content/aip/journal/jcp/123/13/10.1063/1.2034507
2005-09-30
2014-04-20
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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Effects of C–H stretch excitation on the H+CH4 reaction
http://aip.metastore.ingenta.com/content/aip/journal/jcp/123/13/10.1063/1.2034507
10.1063/1.2034507
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