Determining reaction pathways at low temperatures by isotopic substitution: the case of BeD (+) + H2O

Yang, Tiangang1,2; Zhao, Bin3; Chen, Gary K.1; Guo, Hua4; Campbell, Wesley C.1,5,6; Hudson, Eric R.1,5,6

2021-11-01

10.1088/1367-2630/ac2ae3

NEW JOURNAL OF PHYSICS   影响因子和分区

1367-2630

Trapped Be+ ions are a leading platform for quantum information science (Gaebler et al 2016 Phys. Rev. Lett. ), but reactions with background gas species, such as H-2 and H2O, result in qubit loss. Our experiment reveals that the BeOH+ ion is the final trapped ion species when both H-2 and H2O exist in a vacuum system with cold, trapped Be+. The BeH+ product in the Be+ + H-2 reaction further reacts with H2O to form BeOH+. To understand the loss mechanism, low-temperature reactions between sympathetically cooled BeD+ ions and H2O molecules have been investigated using an integrated, laser-cooled Be+ ion trap and high-resolution time-of-flight mass spectrometer (Schneider et al 2014 Phys. Rev. Appl. ). Among all the possible products, BeH2O+, H2DO+, BeOD+, and BeOH+, only the BeOH+ molecular ion was observed experimentally, with the assumed co-product of HD. Theoretical analyses based on explicitly correlated restricted coupled cluster singles, doubles, and perturbative triples (RCCSD(T)-F12) method with the augmented correlation-consistent polarized triple zeta (AVTZ) basis set reveal that two intuitive direct abstraction product channels, Be + H2DO+ and D + BeH2O+, are not energetically accessible at the present reaction temperature (similar to 150 K). Instead, a double displacement BeOH+ + HD product channel is accessible due to a large exothermicity of 1.885 eV through a submerged barrier in the reaction pathway. While the BeOD+ + H-2 product channel has a similar exothermicity, the reaction pathway is dynamically unfavourable, as suggested by a sudden vector projection analysis. This work sheds light on the origin of the loss and contaminations of the laser-cooled Be+ ions in quantum-information experiments.

trapped ions quantum information cold reactions

SCI ; EI

英语

通讯

Air Force Office of Scientific Research["FA9550-16-1-0018","FA9550-20-1-0323","FA9550-18-1-0413"] ; Guangdong Innovative & Entrepreneurial Research Team Program[2019ZT08L455] ; National Natural Science Foundation of China (NSFC Center for Chemical Dynamics)[22003023]

Physics

Physics, Multidisciplinary

WOS:000712060000001

IOP Publishing Ltd

20214611162667

Laser cooling ; Mass spectrometers ; Numerical methods ; Temperature ; Trapped ions

Thermodynamics:641.1 ; Light/Optics:741.1 ; Laser Applications:744.9 ; Numerical Methods:921.6 ; Atomic and Molecular Physics:931.3 ; Quantum Theory; Quantum Mechanics:931.4

PHYSICS

Web of Science

1.Univ Calif Los Angeles, Dept Phys & Astron, Los Angeles, CA 90095 USA
2.Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Peoples R China
3.Univ Bielefeld, Fak Chem, Theoret Chem, Univ Str 25, D-33615 Bielefeld, Germany
4.Univ New Mexico, Dept Chem & Chem Biol, Albuquerque, NM 87131 USA
5.Univ Calif Los Angeles, UCLA Ctr Quantum Sci & Engn, Los Angeles, CA 90095 USA
6.Univ Calif Los Angeles, UCLA Challenge Inst Quantum Computat, Los Angeles, CA 90095 USA

Yang, Tiangang,Zhao, Bin,Chen, Gary K.,et al. Determining reaction pathways at low temperatures by isotopic substitution: the case of BeD (+) + H2O[J]. NEW JOURNAL OF PHYSICS,2021,23(11).

Yang, Tiangang,Zhao, Bin,Chen, Gary K.,Guo, Hua,Campbell, Wesley C.,&Hudson, Eric R..(2021).Determining reaction pathways at low temperatures by isotopic substitution: the case of BeD (+) + H2O.NEW JOURNAL OF PHYSICS,23(11).

Yang, Tiangang,et al."Determining reaction pathways at low temperatures by isotopic substitution: the case of BeD (+) + H2O".NEW JOURNAL OF PHYSICS 23.11(2021).