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Title: The geometric phase controls ultracold chemistry

Abstract

In this study, the geometric phase is shown to control the outcome of an ultracold chemical reaction. The control is a direct consequence of the sign change on the interference term between two scattering pathways (direct and looping), which contribute to the reactive collision process in the presence of a conical intersection (point of degeneracy between two Born–Oppenheimer electronic potential energy surfaces). The unique properties of the ultracold energy regime lead to an effective quantization of the scattering phase shift enabling maximum constructive or destructive interference between the two pathways. By taking the O + OH → H + O2 reaction as an illustrative example, it is shown that inclusion of the geometric phase modifies ultracold reaction rates by nearly two orders of magnitude. Interesting experimental control possibilities include the application of external electric and magnetic fields that might be used to exploit the geometric phase effect reported here and experimentally switch on or off the reactivity.

Authors:
 [1];  [2];  [2]
+ Show Author Affiliations
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. Univ. of Nevada, Las Vegas, NV (United States)
Publication Date:
Research Org.:
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1235941
Report Number(s):
LA-UR-15-24052
Journal ID: ISSN 2041-1723; ncomms8918; TRN: US1600419
Grant/Contract Number:  
AC52-06NA25396
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 6; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; chemical sciences; physical chemistry; atomic and molecular physics; theoretical physics

Citation Formats

Kendrick, B. K., Hazra, Jisha, and Balakrishnan, N. The geometric phase controls ultracold chemistry. United States: N. p., 2015. Web. doi:10.1038/ncomms8918.
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Kendrick, B. K., Hazra, Jisha, & Balakrishnan, N. The geometric phase controls ultracold chemistry. United States. https://doi.org/10.1038/ncomms8918
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Kendrick, B. K., Hazra, Jisha, and Balakrishnan, N. Thu . "The geometric phase controls ultracold chemistry". United States. https://doi.org/10.1038/ncomms8918. https://www.osti.gov/servlets/purl/1235941.
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@article{osti_1235941,
title = {The geometric phase controls ultracold chemistry},
author = {Kendrick, B. K. and Hazra, Jisha and Balakrishnan, N.},
abstractNote = {In this study, the geometric phase is shown to control the outcome of an ultracold chemical reaction. The control is a direct consequence of the sign change on the interference term between two scattering pathways (direct and looping), which contribute to the reactive collision process in the presence of a conical intersection (point of degeneracy between two Born–Oppenheimer electronic potential energy surfaces). The unique properties of the ultracold energy regime lead to an effective quantization of the scattering phase shift enabling maximum constructive or destructive interference between the two pathways. By taking the O + OH → H + O2 reaction as an illustrative example, it is shown that inclusion of the geometric phase modifies ultracold reaction rates by nearly two orders of magnitude. Interesting experimental control possibilities include the application of external electric and magnetic fields that might be used to exploit the geometric phase effect reported here and experimentally switch on or off the reactivity.},
doi = {10.1038/ncomms8918},
journal = {Nature Communications},
number = ,
volume = 6,
place = {United States},
year = {Thu Jul 30 00:00:00 EDT 2015},
month = {Thu Jul 30 00:00:00 EDT 2015}
}
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https://doi.org/10.1038/ncomms8918
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journal, February 2006

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  • The Journal of Chemical Physics, Vol. 124, Issue 8
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Effect of the geometric phase on nuclear dynamics at a conical intersection: Extension of a recent topological approach from one to two coupled surfaces
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Geometric phase for collinear conical intersections. I. Geometric phase angle and vector potentials
journal, February 2011

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Quantum reactive scattering in three dimensions using hyperspherical (APH) coordinates. Theory
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journal, October 2013

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  • The Journal of Chemical Physics, Vol. 139, Issue 14
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Chemical reaction versus vibrational quenching in low energy collisions of vibrationally excited OH with O
journal, November 2013

  • Pradhan, G. B.; Juanes-Marcos, J. C.; Balakrishnan, N.
  • The Journal of Chemical Physics, Vol. 139, Issue 19
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Quantum dynamics study on the CHIPR potential energy surface for the hydroperoxyl radical: The reactions O + OH⇋O 2 + H
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Strong geometric-phase effects in the hydrogen-exchange reaction at high collision energies: II. Quasiclassical trajectory analysis
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Cold and ultracold molecules: science, technology and applications
journal, May 2009

Interactions and dynamics in Li + Li_2 ultracold collisions
text, January 2007

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    • Nature Communications, Vol. 8, Issue 1
    • DOI: 10.1038/ncomms15897

    Observation of pendular butterfly Rydberg molecules
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