Spectroscopic measurements of the reaction H3+ + H2  H2 + H3+

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Presentation transcript:

Spectroscopic measurements of the reaction H3+ + H2  H2 + H3+ Kyle N. Crabtree, Carrie A. Kauffman, Brian A. Tom, Eftalda Becka, Brett A. McGuire, Benjamin J. McCall University of Illinois

66th OSU International Symposium on Molecular Spectroscopy H3+ + H2  H2 + H3+ H3+ + H2 reaction important for thermalization of H3+ in interstellar clouds (see TF09, 160 MA, 3:52 pm) 1 “identity” H5+ 3 “hop” para-H3+ ortho-H3+ 1/2 3/2 a = kH/kE 6 “exchange” 20 June 2011 66th OSU International Symposium on Molecular Spectroscopy

Previous experimental work M. Cordonnier et al., J. Chem. Phys. (2000), 113, 3181-3193. a = 2.4 + 0.6 @ 400 K 20 June 2011 66th OSU International Symposium on Molecular Spectroscopy

Other experimental work hop exch hop:exchange Experimental data a increases with increasing T temperature 20 June 2011 66th OSU International Symposium on Molecular Spectroscopy

66th OSU International Symposium on Molecular Spectroscopy Experimental setup 20 June 2011 66th OSU International Symposium on Molecular Spectroscopy

66th OSU International Symposium on Molecular Spectroscopy Hollow cathode cell 20 June 2011 66th OSU International Symposium on Molecular Spectroscopy

66th OSU International Symposium on Molecular Spectroscopy Target transitions R(3,0) 2930.1 cm-1 R(3,1)u 2928.3 cm-1 R(3,2)u 2923.3 cm-1 R(3,3)l 2829.9 cm-1 R(2,1)u 2826.1 cm-1 Kinetic and rotational temperature p-H3+ fraction (p3) R(2,2)l 2762.1 cm-1 R(1,0) 2725.9 cm-1 R(1,1)u 2726.2 cm-1 20 June 2011 66th OSU International Symposium on Molecular Spectroscopy

H3+ pressure dependence Uncooled cell (350 K) Liquid N2 cooled cell (135 K) Decrease in H3+ number density with increasing pressure 3-body collisions (H3+ + 2H2  H5+ + H2) To measure hop:exchange ratio of the bimolecular H3+ + H2 reaction, measure p3 as a function of p2 at two pressures for each temperature 20 June 2011 66th OSU International Symposium on Molecular Spectroscopy

H3+/H2 para fraction relationships Uncooled cell (350 K) Liquid N2 cooled cell (135 K) 2-body HT 3-body HT Low temperature 20 June 2011 66th OSU International Symposium on Molecular Spectroscopy

Uncooled plasma (350 K) fit No evidence for influence of nuclear-spin-dependent 3-body collisions in data 20 June 2011 66th OSU International Symposium on Molecular Spectroscopy

Liquid N2 cooled plasma (135 K) modeling Tkin = 135 K 20 June 2011 66th OSU International Symposium on Molecular Spectroscopy

Summary of experimental data T = 450 K a decreases with temperature: 1.6 at 350 K down to 0.5 at 135 K 20 June 2011 66th OSU International Symposium on Molecular Spectroscopy

66th OSU International Symposium on Molecular Spectroscopy H3+ + H2  H2 + H3+ 1 “identity” H5+ 3 “hop” 6 “exchange” 20 June 2011 66th OSU International Symposium on Molecular Spectroscopy

Dynamics of Reaction D2d C2v C2v hop exchange PES: Z. Xie, B. J. Braams, & J. M. Bowman, J. Chem. Phys. (2005) 122, 224307. D2d 3000 cm-1 C2v 1500 cm-1 50 cm-1 C2v hop exchange Hop is dynamically faster than exchange; short complex lifetime favors hop At low temperatures, “statistical” hop/exchange = 0.5 seems valid 20 June 2011 66th OSU International Symposium on Molecular Spectroscopy

66th OSU International Symposium on Molecular Spectroscopy Acknowledgements Kisam Park More information: Tomorrow, TF09, 160 MA K. N. Crabtree, B. A. Tom, B. J. McCall, J. Chem. Phys. (2011) 134, 194310. K. N. Crabtree et al., J. Chem. Phys. (2011) 134, 194311. http://bjm.scs.illinois.edu 20 June 2011 66th OSU International Symposium on Molecular Spectroscopy