High resolution electronic spectroscopy of uranium mononitride, UN

Le, Anh T.; Bai, Xi-lin; Heaven, Michael C.; Steimle, Timothy C.

doi:10.1063/5.0157884

High resolution electronic spectroscopy of uranium mononitride, UN

Journal Article · Thu Jun 22 00:00:00 EDT 2023 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/5.0157884· OSTI ID:2418930

Le, Anh T. ^[1]; Bai, Xi-lin ^[2]; ^[3]; ^[4]

Georgia Institute of Technology, Atlanta, GA (United States)
Shanxi Normal University, Linfen (China)
Emory Univ., Atlanta, GA (United States)
Arizona State Univ., Tempe, AZ (United States)

The isoelectronic molecules UN and UO⁺ are known to have Ω = 3.5 and Ω = 4.5 ground states, respectively (where Ω is the unsigned projection of the electronic angular momentum along the internuclear axis). A ligand field theory model has been proposed to account for the difference [Matthew and Morse, J. Chem. Phys. 138, 184303 (2013)]. The ground state of UO⁺ arises from the U³⁺(5f³(⁴I_4.5))O²⁻ configuration. Owing to the higher nominal charge of the N³⁻ ligand, the U³⁺ ion in UN is stabilized by promoting one of the 5f electrons to the more polarizable 7s orbital, reducing the repulsive interaction with the ligand and rendering U³⁺(5f²7s(⁴H_3.5))N³⁻ the lowest energy configuration. In the present work, we have advanced the characterization of the UN ground state through studies of two electronic transitions, [18.35]4.5-X(1)3.5 and [18.63]4.5-X(1)3.5, using sub-Doppler laser excitation techniques with fluorescence detection. Further, spectra were recorded under field-free conditions and in the presence of static electric or magnetic fields. The ground state electric dipole moment [μ = 4.30(2) D] and magnetic g_e-factor [2.160(9)] were determined from these data. These values were both consistent with the 5f²7s configurational assignment. Dispersed fluorescence measurements were used to determine vibrational constants for the ground and first electronically excited states. Electric dipole moments and magnetic g_e-factors are also reported for the higher-energy electronically excited states.

View Accepted Manuscript (DOE)

Research Organization:: Emory Univ., Atlanta, GA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: FG02-01ER15153

OSTI ID:: 2418930

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 24 Vol. 158; ISSN 1089-7690; ISSN 0021-9606

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

Country of Publication:: United States

Language:: English

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