Spin–orbit coupling of electrons on separate lanthanide atoms of Pr2O2 and its singly charged cation

Nakamura, Taiji; Dangi, Beni B.; Wu, Lu; Zhang, Yuchen; Schoendorff, George; Gordon, Mark S.; Yang, Dong-Sheng

doi:10.1063/5.0185579

Title: Spin–orbit coupling of electrons on separate lanthanide atoms of Pr₂O₂ and its singly charged cation

Journal Article · 21 December 2023 · Journal of Chemical Physics

DOI: https://doi.org/10.1063/5.0185579 · OSTI ID:2305638

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^[2]; Wu, Lu ^[2]; Zhang, Yuchen ^[2];

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Iowa State Univ., Ames, IA (United States); Kyushu Univ., Fukuoka (Japan)
Univ. of Kentucky, Lexington, KY (United States)
Ames Lab., and Iowa State Univ., Ames, IA (United States); Air Force Research Lab. (AFRL), Edwards Air Force Base, CA (United States)
Ames Lab., and Iowa State Univ., Ames, IA (United States)

Although it plays a critical role in the photophysics and catalysis of lanthanides, spin–orbit coupling of electrons on individual lanthanide atoms in small clusters is not well understood. The major objective of this work is to probe such coupling of the praseodymium (Pr) 4f and 6s electrons in Pr₂O₂ and Pr₂O₂+. The approach combines mass-analyzed threshold ionization spectroscopy and spin–orbit multiconfiguration second-order quasi-degenerate perturbation theory. The energies of six ionization transitions are precisely measured; the adiabatic ionization energy of the neutral cluster is 38 045 (5) cm^–1. Most of the electronic states involved in these transitions are identified as spin–orbit coupled states consisting of two or more electron spins. The electron configurations of these states are 4f⁴6s² for the neutral cluster and 4^f46^s for the singly charged cation, both in planar rhombus-type structures. Finally, the spin–orbit splitting due to the coupling of the electrons on the separate Pr atoms is on the order of hundreds of wavenumbers.

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Research Organization:: Ames Laboratory (AMES), Ames, IA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

OSTI ID:: 2305638

Alternate ID(s):: OSTI ID: 2375395

Report Number(s):: IS-J--11,234

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 24 Vol. 159; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Spin–orbit coupling of electrons on separate lanthanide atoms of Pr2O2 and its singly charged cation

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Title: Spin–orbit coupling of electrons on separate lanthanide atoms of Pr₂O₂ and its singly charged cation