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

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

doi:10.1063/5.0185579

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

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

Producción científica: Article › revisión exhaustiva

7 Citas (Scopus)

Resumen

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 4f⁴6s for the singly charged cation, both in planar rhombus-type structures. The spin-orbit splitting due to the coupling of the electrons on the separate Pr atoms is on the order of hundreds of wavenumbers.

Idioma original	English
Número de artículo	244303
Publicación	Journal of Chemical Physics
Volumen	159
N.º	24
DOI	https://doi.org/10.1063/5.0185579
Estado	Published - dic 28 2023

Nota bibliográfica

Publisher Copyright:
© 2023 Author(s).

Financiación

This material was based upon work supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences, Chemical Physics Program (Award No. DE-SC0021227) (D.-S.Y.). G.S., T.N., and M.S.G. were supported by the Department of Energy (Grant No. AL-20-380-066), administered by the Ames Laboratory, which is operated by Iowa State University under Contract No. DE-AC02-07CH11338. This research was performed while G.S. held an NRC Research Associateship award at the Air Force Research Laboratory in conjunction with the AFRL Science and Technology Fellowship Program. This material was based upon work supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences, Chemical Physics Program (Award No. DE-SC0021227) (D.-S.Y.). G.S., T.N., and M.S.G. were supported by the Department of Energy (Grant No. AL-20-380-066), administered by the Ames Laboratory, which is operated by Iowa State University under Contract No. DE-AC02-07CH11338. This research was performed while G.S. held an NRC Research Associateship award at the Air Force Research Laboratory in conjunction with the AFRL Science and Technology Fellowship Program.

Financiadores	Número del financiador
Ames Laboratory Chemical Physics program	DE-SC0021227
U.S. Department of Energy Oak Ridge National Laboratory U.S. Department of Energy National Science Foundation National Energy Research Scientific Computing Center	AL-20-380-066
U.S. Department of Energy Oak Ridge National Laboratory U.S. Department of Energy National Science Foundation National Energy Research Scientific Computing Center
DOE Basic Energy Sciences
Air Force Research Laboratory
Ames Laboratory	DE-AC02-07CH11338
Ames Laboratory
Chemical Sciences, Geosciences, and Biosciences Division

ASJC Scopus subject areas

General Physics and Astronomy
Physical and Theoretical Chemistry

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10.1063/5.0185579

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abstract = "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 4f46s for the singly charged cation, both in planar rhombus-type structures. 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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AU - Nakamura, Taiji

AU - Dangi, Beni B.

AU - Wu, Lu

AU - Zhang, Yuchen

AU - Schoendorff, George

AU - Gordon, Mark S.

AU - Yang, Dong Sheng

PY - 2023/12/28

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AB - 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 4f46s for the singly charged cation, both in planar rhombus-type structures. 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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