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Title: Geometric phase effects in the ultracold H + H2 reaction

Journal Article · · Journal of Chemical Physics
DOI:https://doi.org/10.1063/1.4966037· OSTI ID:1330279
 [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
+ Show Author Affiliations

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.

Research Organization:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Organization:
USDOE Laboratory Directed Research and Development (LDRD) Program
Grant/Contract Number:
20140309ER; AC52-06NA25396
OSTI ID:
1330279
Alternate ID(s):
OSTI ID: 1345165; OSTI ID: 1416459
Report Number(s):
LA-UR-16-25624; JCPSA6; 10.1063/1.4966037
Journal Information:
Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Vol. 145 Journal Issue: 16; ISSN 0021-9606
Publisher:
American Institute of PhysicsCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 15 works
Citation information provided by
Web of Science

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Non-adiabatic quantum reactive scattering in hyperspherical coordinates journal January 2018

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
astronomy and astrophysics
inorganic and physical chemistry
ultracold chemistry
hydrogen reaction