Geometric phase effects in the ultracold H + H2 reaction
Abstract
The H3 system has served as a prototype for geometric phase (GP) effects in bimolecular chemical reactions for over three decades. Despite a large number of theoretical and experimental efforts, no conclusive evidence of GP effects in the integral cross section or reaction rate has been presented until recently. Here we report a more detailed account of GP effects in the H + H2(v = 4, j = 0) → H + H2(v', j') (para-para) reaction rate coefficients for temperatures between 1 μK (8.6 × 10–11 eV) and 100 K (8.6 × 10–3 eV). The GP effect is found to persist in both vibrationally resolved and total rate coefficients for collision energies up to about 10 K. The GP effect also appears in rotationally resolved differential cross sections leading to a very different oscillatory structure in both energy and scattering angle. It is shown to suppress a prominent shape resonance near 1 K and enhance a shape resonance near 8 K, providing new experimentally verifiable signatures of the GP effect in the fundamental hydrogen exchange reaction. As a result, the GP effect in the D + D2 and T + T2 reactions is also examined in the ultracold limit andmore »
- Authors:
-
- Theoretical Division (T-1, MS B221), Los Alamos National Laboratory, Los Alamos, New Mexico 87545, USA
- Department of Chemistry, University of Nevada, Las Vegas, Nevada 89154, USA
- Publication Date:
- Research Org.:
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE Laboratory Directed Research and Development (LDRD) Program
- OSTI Identifier:
- 1330279
- Alternate Identifier(s):
- OSTI ID: 1345165; OSTI ID: 1416459
- Report Number(s):
- LA-UR-16-25624
Journal ID: ISSN 0021-9606; JCPSA6; 10.1063/1.4966037
- Grant/Contract Number:
- 20140309ER; AC52-06NA25396
- Resource Type:
- Published Article
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Name: Journal of Chemical Physics Journal Volume: 145 Journal Issue: 16; Journal ID: ISSN 0021-9606
- Publisher:
- American Institute of Physics
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; astronomy and astrophysics; inorganic and physical chemistry; ultracold chemistry; hydrogen reaction
Citation Formats
Kendrick, B. K., Hazra, Jisha, and Balakrishnan, N. Geometric phase effects in the ultracold H + H2 reaction. United States: N. p., 2016.
Web. doi:10.1063/1.4966037.
Kendrick, B. K., Hazra, Jisha, & Balakrishnan, N. Geometric phase effects in the ultracold H + H2 reaction. United States. https://doi.org/10.1063/1.4966037
Kendrick, B. K., Hazra, Jisha, and Balakrishnan, N. Thu .
"Geometric phase effects in the ultracold H + H2 reaction". United States. https://doi.org/10.1063/1.4966037.
@article{osti_1330279,
title = {Geometric phase effects in the ultracold H + H2 reaction},
author = {Kendrick, B. K. and Hazra, Jisha and Balakrishnan, N.},
abstractNote = {The H3 system has served as a prototype for geometric phase (GP) effects in bimolecular chemical reactions for over three decades. Despite a large number of theoretical and experimental efforts, no conclusive evidence of GP effects in the integral cross section or reaction rate has been presented until recently. Here we report a more detailed account of GP effects in the H + H2(v = 4, j = 0) → H + H2(v', j') (para-para) reaction rate coefficients for temperatures between 1 μK (8.6 × 10–11 eV) and 100 K (8.6 × 10–3 eV). The GP effect is found to persist in both vibrationally resolved and total rate coefficients for collision energies up to about 10 K. The GP effect also appears in rotationally resolved differential cross sections leading to a very different oscillatory structure in both energy and scattering angle. It is shown to suppress a prominent shape resonance near 1 K and enhance a shape resonance near 8 K, providing new experimentally verifiable signatures of the GP effect in the fundamental hydrogen exchange reaction. As a result, the GP effect in the D + D2 and T + T2 reactions is also examined in the ultracold limit and its sensitivity to the potential energy surface is explored.},
doi = {10.1063/1.4966037},
journal = {Journal of Chemical Physics},
number = 16,
volume = 145,
place = {United States},
year = {Thu Oct 27 00:00:00 EDT 2016},
month = {Thu Oct 27 00:00:00 EDT 2016}
}
https://doi.org/10.1063/1.4966037
Web of Science
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Works referencing / citing this record:
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