Spectroscopic Measurements of the Reaction H_3^+ + H_2 → H_2 + H_3^+

Details Spectroscopic Measurements of the Reaction H_3^+ + H_2 → H_2 + H_3^+ Spectroscopic Measurements of the Reaction H_3^+ + H_2 → H_2 + H_3^+

Jun 2011

adsabs.harvard.edu/cgi-bin/nph-data_query?bibcode=2011mss..confemi03c&link_type=abstract

"International Symposium On Molecular Spectroscopy, 66th Meeting, Held 20-24 June, 2011 at Ohio State University. http://molspec

Computer Science

Radicals And Ions

Scientific paper

The fundamental reaction involving H_3^+ and H_2 has not been well-studied in the laboratory. Typical approaches to studying kinetics using mass spectrometry are ineffective because the products have identical masses to the reactants. Isotopic labeling fundamentally alters the exchange symmetry of this system, and therefore cannot be employed. However, because the two nuclear spin configurations of H_3^+ (ortho, I=3/2, and para, I=1/2) and H_2 (ortho, I=1, and para, I=0) are linked to specific rotational states by symmetry, spectroscopy is a useful tool for studying this reaction. We have employed infrared multipass direct absorption spectroscopy to measure transitions in the νb{2} fundamental band of H_3^+ using a difference frequency generation laser. Hydrogenic plasmas were produced in a hollow cathode discharge cell, which could be cooled as low as 130 K using liquid nitrogen. To measure the nuclear spin dependence of the H_3^+ + H_2 reaction, we prepared hydrogen gas enriched up to 99.9% para-H_2 using a para-hydrogen converter, and determined the ortho:para ratio of H_3^+ formed in the hollow cathode plasma at steady state as a function of both para-hydrogen enrichment and temperature. By utilizing steady state chemical models, we have determined that the ratio of the rates of the proton hop and hydrogen exchange pathways (α ≡ k^H/k^E) decreases from 1.6±0.1 at 350 K to 0.5±0.1 at 135 K. These results suggest that at lower temperatures, the intermediate (H_5^+)^* complex lifetime increases, leading to more statistical proton scrambling.

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