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Title: The geometric phase controls ultracold chemistry

Journal Article · · Nature Communications
DOI:https://doi.org/10.1038/ncomms8918· OSTI ID:1235941
 [1];  [2];  [2]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. Univ. of Nevada, Las Vegas, NV (United States)

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.

Research Organization:
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Sponsoring Organization:
USDOE
Grant/Contract Number:
AC52-06NA25396
OSTI ID:
1235941
Report Number(s):
LA-UR-15-24052; ncomms8918; TRN: US1600419
Journal Information:
Nature Communications, Vol. 6; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 62 works
Citation information provided by
Web of Science

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Atom-molecule collisions, spin relaxation, and sympathetic cooling in an ultracold spin-polarized Rb ( S 2 ) SrF ( Σ + 2 ) mixture journal October 2018
Topological classification of molecules and chemical reactions with a perplectic structure journal January 2020
Modulating hydrogen diffusion on metal surfaces by nonadiabatic transitions journal June 2019
Geometric phase from Aharonov–Bohm to Pancharatnam–Berry and beyond journal June 2019
Several levels of theory for description of isotope effects in ozone: Effect of resonance lifetimes and channel couplings journal October 2018
Non-adiabatic quantum reactive scattering in hyperspherical coordinates journal January 2018
Geometric phase effects on photodissociation dynamics of diatomics journal December 2018
Quantum wavepacket method for state-to-state reactive cross sections in hyperspherical coordinates journal November 2018
Universality and chaoticity in ultracold K+KRb chemical reactions journal July 2017
Observation of pendular butterfly Rydberg molecules journal October 2016
Quantum ergodicity and energy flow in molecules journal July 2015
Observation of pendular butterfly Rydberg molecules text January 2016