DOI: 10.1063/1.465312. The reaction of argon ions with hydrogen and deuterium molecules by crossed beams: Low energy resonances and role of vibronic levels of the intermediate complex

The reaction of argon ions with hydrogen and deuterium molecules by crossed beams: Low energy resonances and role of vibronic levels of the intermediate complex

10.1063/1.465312

Crossref journal-article

AIP Publishing

The Journal of Chemical Physics (317)

Abstract

In a crossed beam experiment, cross sections have been measured for the ion–molecule reactions Ar++H2→ArH++H and Ar++D2→ArD++D. Low collision energies (0.025≤E≤ 1 eV) and high resolution (ΔE∼10 meV, half-width at half-maximum) have been obtained using the method of guiding the ion beam by an octopole field and the technique of supersonic beams for H2 or D2. A structure in the energy dependence of cross sections has been found and attributed to a manifestation of vibronic resonances. Calculations are presented and compared to experimental findings to illustrate this effect, which arises because of the successive population of vibronic levels of the charge transfer complex Ar–H2+ or Ar–D2+, which are the intermediates for these reactions. Empirical potential energy surfaces for the entrance channels have been constructed accounting explicitly for the open shell nature and spin–orbit effects in Ar+(2PJ); symmetry considerations have also been used to establish the sequence of pertinent vibronic surfaces of the charge transfer intermediate complex—the role of configuration interaction in the latter is also discussed. The reaction dynamics has been treated as a sequence of nonadiabatic transitions at crossings of potential energy surfaces—quantum mechanical tunneling has been found crucial for the proper description of the observed energy dependence of the cross sections and the vibronic resonance structure. A higher frequency structure, borne out by the calculations and due to a manifold of metastable states supported by the vibronic levels of the intermediate charge transfer complex, appears to be washed out by the finite experimental resolution. It is also shown that finite experimental resolution had been the reason for the failure of detecting vibronic resonances in previous experiments and that the present ones are in general agreement with them when resolution is artificially lowered. Finally, it is pointed out that the present approach, when applied to charge transfer processes, provides a model which appears consistent with existing measurements. It also accounts for the observed selective reactivity of the fine structure components of argon ions.

Bibliography

Tosi, P., Dmitrijev, O., Soldo, Y., Bassi, D., Cappelletti, D., Pirani, F., & Aquilanti, V. (1993). The reaction of argon ions with hydrogen and deuterium molecules by crossed beams: Low energy resonances and role of vibronic levels of the intermediate complex. The Journal of Chemical Physics, 99(2), 985â1003.

Authors 7

Paolo Tosi (first)
Oleg Dmitrijev (additional)
Yvonne Soldo (additional)
Davide Bassi (additional)
David Cappelletti (additional)
Fernando Pirani (additional)
Vincenzo Aquilanti (additional)

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Dates

Type	When
Created	23 years ago (July 26, 2002, 8:22 a.m.)
Deposited	1 year, 6 months ago (Feb. 6, 2024, 3:07 a.m.)
Indexed	1 month, 2 weeks ago (July 8, 2025, 6:26 a.m.)
Issued	32 years, 1 month ago (July 15, 1993)
Published	32 years, 1 month ago (July 15, 1993)
Published Print	32 years, 1 month ago (July 15, 1993)

Funders 0

None

BibTeX

@article{Tosi_1993, title={The reaction of argon ions with hydrogen and deuterium molecules by crossed beams: Low energy resonances and role of vibronic levels of the intermediate complex}, volume={99}, ISSN={1089-7690}, url={http://dx.doi.org/10.1063/1.465312}, DOI={10.1063/1.465312}, number={2}, journal={The Journal of Chemical Physics}, publisher={AIP Publishing}, author={Tosi, Paolo and Dmitrijev, Oleg and Soldo, Yvonne and Bassi, Davide and Cappelletti, David and Pirani, Fernando and Aquilanti, Vincenzo}, year={1993}, month=jul, pages={985–1003} }

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  "abstract": "<jats:p>In a crossed beam experiment, cross sections have been measured for the ion\u2013molecule reactions Ar++H2\u2192ArH++H and Ar++D2\u2192ArD++D. Low collision energies (0.025\u2264E\u2264 1 eV) and high resolution (\u0394E\u223c10 meV, half-width at half-maximum) have been obtained using the method of guiding the ion beam by an octopole field and the technique of supersonic beams for H2 or D2. A structure in the energy dependence of cross sections has been found and attributed to a manifestation of vibronic\u2008resonances. Calculations are presented and compared to experimental findings to illustrate this effect, which arises because of the successive population of vibronic levels of the charge transfer complex Ar\u2013H2+ or Ar\u2013D2+, which are the intermediates for these reactions. Empirical potential energy surfaces for the entrance channels have been constructed accounting explicitly for the open shell nature and spin\u2013orbit effects in Ar+(2PJ); symmetry considerations have also been used to establish the sequence of pertinent vibronic surfaces of the charge transfer intermediate complex\u2014the role of configuration interaction in the latter is also discussed. The reaction dynamics has been treated as a sequence of nonadiabatic transitions at crossings of potential energy surfaces\u2014quantum mechanical tunneling has been found crucial for the proper description of the observed energy dependence of the cross sections and the vibronic resonance structure. A higher frequency structure, borne out by the calculations and due to a manifold of metastable states supported by the vibronic levels of the intermediate charge transfer complex, appears to be washed out by the finite experimental resolution. It is also shown that finite experimental resolution had been the reason for the failure of detecting vibronic resonances in previous experiments and that the present ones are in general agreement with them when resolution is artificially lowered. Finally, it is pointed out that the present approach, when applied to charge transfer processes, provides a model which appears consistent with existing measurements. It also accounts for the observed selective reactivity of the fine structure components of argon ions.</jats:p>",
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