Non-adiabatic quantum reactive scattering calculations for the ultracold hydrogen exchange reaction: H + H _{2}( $v=4-8,\phantom{\rule{0ex}{0ex}}j=0$) $\to $ H + H _{2}( ${v}^{\text{'}},\phantom{\rule{0ex}{0ex}}{j}^{\text{'}}$)
A non-adiabatic quantum dynamics methodology based on a time-independent coupled-channel approach is applied to the fully symmetric H + H _{2}( $v=4-8,\phantom{\rule{0ex}{0ex}}j=0$) $\to $ H + H _{2}( ${v}^{\text{'}},\phantom{\rule{0ex}{0ex}}{j}^{\text{'}}$) reaction for the first time. A two-state diabatic representation is used which includes the effects of the geometric phase (GP) and other non-adiabatic couplings. Ultracold rate coefficients are reported as a function of collision energy between $1\phantom{\rule{0ex}{0ex}}\mathrm{\mu}\text{K}$ and $100\phantom{\rule{0ex}{0ex}}\text{K}$. A second set of adiabatic calculations are also performed both with and without the GP. The results for $v>4$ are reported here for the first time and a new experimentally detectable signature of the GP is discovered associated with the dramatic appearance of an $l=1$ shape resonance near $1\phantom{\rule{0ex}{0ex}}\text{K}$ in the total rate coefficient for $v=6$ which is absent for $v=4$ and 5.
- Publication Date:
- Report Number(s):
- LA-UR-18-23192
Journal ID: ISSN 0301-0104
- Grant/Contract Number:
- AC52-06NA25396
- Type:
- Accepted Manuscript
- Journal Name:
- Chemical Physics
- Additional Journal Information:
- Journal Name: Chemical Physics; Journal ID: ISSN 0301-0104
- Publisher:
- Elsevier
- Research Org:
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Sponsoring Org:
- USDOE National Nuclear Security Administration (NNSA); LANL Laboratory Directed Research and Development (LDRD) Program
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; non-adiabatic dynamics; geometric phase; reactive scattering; ultracold chemistry; quantum dynamics; cold molecules
- OSTI Identifier:
- 1459826
Kendrick, Brian K. Non-adiabatic quantum reactive scattering calculations for the ultracold hydrogen exchange reaction: H + H2(v=4-8,j=0) → H + H2(v',j'). United States: N. p.,
Web. doi:10.1016/j.chemphys.2018.07.001.
Kendrick, Brian K. Non-adiabatic quantum reactive scattering calculations for the ultracold hydrogen exchange reaction: H + H2(v=4-8,j=0) → H + H2(v',j'). United States. doi:10.1016/j.chemphys.2018.07.001.
Kendrick, Brian K. 2018.
"Non-adiabatic quantum reactive scattering calculations for the ultracold hydrogen exchange reaction: H + H2(v=4-8,j=0) → H + H2(v',j')". United States.
doi:10.1016/j.chemphys.2018.07.001. https://www.osti.gov/servlets/purl/1459826.
@article{osti_1459826,
title = {Non-adiabatic quantum reactive scattering calculations for the ultracold hydrogen exchange reaction: H + H2(v=4-8,j=0) → H + H2(v',j')},
author = {Kendrick, Brian K.},
abstractNote = {A non-adiabatic quantum dynamics methodology based on a time-independent coupled-channel approach is applied to the fully symmetric H + H2(v=4-8,j=0) → H + H2(v',j') reaction for the first time. A two-state diabatic representation is used which includes the effects of the geometric phase (GP) and other non-adiabatic couplings. Ultracold rate coefficients are reported as a function of collision energy between 1μK and 100K. A second set of adiabatic calculations are also performed both with and without the GP. The results for v>4 are reported here for the first time and a new experimentally detectable signature of the GP is discovered associated with the dramatic appearance of an l=1 shape resonance near 1K in the total rate coefficient for v=6 which is absent for v=4 and 5.},
doi = {10.1016/j.chemphys.2018.07.001},
journal = {Chemical Physics},
number = ,
volume = ,
place = {United States},
year = {2018},
month = {7}
}