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Updated: Feb 23, 2026

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Rotationally Resolved Electronic Spectroscopy of UO2.

Jiande Han1, Jiayue Lin1, Michael C Heaven1

  • 1Department of Chemistry, Emory University, Atlanta, Georgia 30322, United States.

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|February 21, 2026
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Summary

Rotationally resolved electronic spectra of gas-phase uranium dioxide (UO2) reveal its ground state is X3Φ2u. This study determined vibrational frequencies and bond length, providing insights into UO2 electronic configurations and excited state dynamics.

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Area of Science:

  • Molecular Spectroscopy
  • Quantum Chemistry
  • Inorganic Chemistry

Background:

  • Uranium dioxide (UO2) is a key material in nuclear energy.
  • Understanding its electronic structure and spectroscopy is crucial for safety and efficiency.
  • Previous studies have lacked detailed rotational resolution for gas-phase UO2.

Purpose of the Study:

  • To investigate the electronic structure of gas-phase UO2 using high-resolution spectroscopy.
  • To determine the ground state electronic configuration and vibrational properties.
  • To analyze the dynamics of excited electronic states and fluorescence decay.

Main Methods:

  • Rotationally resolved electronic spectroscopy was employed for gas-phase UO2.
  • Analysis of rotational fine structure identified the ground state as X3Φ2u.
  • Vibrational frequencies and bond length were calculated from spectral data.

Main Results:

  • The ground state of UO2 was confirmed as X3Φ2u, originating from a 5f7s electron configuration.
  • Transitions to excited states [11.51]3g and [17.68]4g were observed and assigned.
  • Ground-state vibrational fundamentals (853(5) and 133(5) cm−1) and bond length (1.781 Å) were determined.
  • Anomalously long fluorescence decay lifetimes (1.5–4.7 μs) were observed for excited states.

Conclusions:

  • The electronic configuration of UO2 ground and excited states was elucidated.
  • Vibrational modes and molecular geometry were characterized.
  • Long fluorescence lifetimes suggest significant mixing with dark vibronic states, impacting UO2 photophysics.