Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

Electronic Configuration Assignments for UO from Electric Dipole Moment Measurements

Journal Article · · Journal of Physical Chemistry Letters
 [1];  [2];  [3];  [4]
  1. Emory Univ., Atlanta, GA (United States); Emory University
  2. Georgia Institute of Technology, Atlanta, GA (United States)
  3. Arizona State Univ., Tempe, AZ (United States)
  4. Emory Univ., Atlanta, GA (United States)
Diatomic UO has more than 48 bound states within 10000 cm-1 of the ground state. This electronic state congestion has been attributed to interleaved states from the electronic configurations U2+($5f^37s$)O2- and U2+($5f^27s^2$)O2-, respectively. Ligand field theory predicts that each electronic configuration will exhibit states with distinguishable, characteristic vibrational and rotational constants. However, vibronic state mixing modifies the observed vibration–rotation constants, leading to uncertainty in the configurational assignments. The permanent electric dipole moment ($$μ_e$$) of an electronic state should also manifest a value that is characteristic of the parent electronic configuration. $$μ_e$$ and other electrostatic and magnetostatic properties should be less influenced by the vibronic state mixing, providing more robust indicators for configurational assignments. In the present study, we have measured the $$μ_e$$ values for four electronic states of UO. Here, the results clearly demonstrate that the ground state (X(1)4) and the first electronically excited state ((2)4) are derived from the U2+($5f^37s$)O2– and U2+($5f^27s^2$)O2– configurations, respectively.
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:
1906282
Journal Information:
Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 46 Vol. 13; ISSN 1948-7185
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

References (25)

Diatomic Molecule Electronic Structure beyond Simple Molecular Constants journal September 1982
The electronic structure of the actinide oxides and their singly and doubly charged cations: A ligand field approach journal December 2020
The ORCA program system: The ORCA program system journal June 2011
Laser Spectroscopy of UO: Characterization and Assignment of States in the 0- to 3-eV Range, with a Comparison to the Electronic Structure of ThO journal March 1994
Electronic Spectroscopy of UO journal September 1997
Rotationally resolved electronic spectra for uranium monoxide journal August 1985
LEVEL: A computer program for solving the radial Schrödinger equation for bound and quasibound levels journal January 2017
Optical spectroscopy and modeling of uranium gas-phase oxidation: Progress and perspectives journal November 2021
Quantum Chemical Calculations and Experimental Investigations of Molecular Actinide Oxides journal January 2015
All-Electron Scalar Relativistic Basis Sets for the Actinides journal February 2011
Theoretical Study of Bond Distances and Dissociation Energies of Actinide Oxides AnO and AnO 2 journal April 2012
Accurate Ionization Potentials for UO and UO 2 :  A Rigorous Test of Relativistic Quantum Chemistry Calculations journal June 2003
Infrared Spectra of UO 2 , UO 2 + , and UO 2 - in Solid Neon journal June 2000
Computed Vibrational Frequencies of Actinide Oxides AnO 0/+/2+ and AnO 2 0/+/2+ (An = Th, Pa, U, Np, Pu, Am, Cm) journal June 2011
Electronic Spectrum of the UO and UO + Molecules journal December 2014
Probing actinide electronic structure using fluorescence and multi-photon ionization spectroscopy journal January 2006
Infrared spectra of matrix‐isolated uranium oxide species. I. The stretching region journal May 1973
Spectroscopy of the ground and low-lying excited states of ThO+ journal February 2006
Probing the electronic structure of UO+ with high-resolution photoelectron spectroscopy journal October 2006
The permanent electric dipole moments and magnetic g factors of uranium monoxide journal November 2006
Gaussian basis sets for use in correlated molecular calculations. I. The atoms boron through neon and hydrogen journal January 1989
Reactions of pulsed‐laser evaporated uranium atoms with molecular oxygen: Infrared spectra of UO, UO 2 , UO 3 , UO 2 + , UO 2 2+ , and UO 3 –O 2 in solid argon journal March 1993
Formation of 238 U 16 O and 238 U 18 O observed by time-resolved emission spectroscopy subsequent to laser ablation journal July 2017
Comparative electronic structure of a lanthanide and actinide diatomic oxide: Nd versus U journal January 2003
High precision description of the rovibronic structure of the I $\mathsf{_2}$ B-X spectrum journal February 2004

Similar Records

High resolution electronic spectroscopy of uranium mononitride, UN
Journal Article · Wed Jun 21 20:00:00 EDT 2023 · Journal of Chemical Physics · OSTI ID:2418930

Laser spectroscopy of UO: Characterization and assignment of states in the 0- to 3-eV range, with a comparison to the electronic structure of ThO
Journal Article · Mon Feb 28 23:00:00 EST 1994 · Journal of Molecular Spectroscopy; (United States) · OSTI ID:7270740

Spectroscopy and electronic structure of the low-energy states of ThN
Journal Article · Wed Feb 03 19:00:00 EST 2021 · Journal of Molecular Spectroscopy · OSTI ID:1849366