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Title: 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 » its sensitivity to the potential energy surface is explored.« less

Authors:
 [1];  [2]; ORCiD logo [2]
  1. Theoretical Division (T-1, MS B221), Los Alamos National Laboratory, Los Alamos, New Mexico 87545, USA
  2. 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}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1063/1.4966037

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Cited by: 15 works
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Works referencing / citing this record:

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