Laser-induced fluorescence experimental spectroscopy and theoretical calculations of uranium monoxide

doi:10.1088/1674-1056/ac43a4

中国物理B ›› 2022, Vol. 31 ›› Issue (5): 53301-053301.doi: 10.1088/1674-1056/ac43a4

Laser-induced fluorescence experimental spectroscopy and theoretical calculations of uranium monoxide

Xi-Lin Bai(白西林)^1,†, Xue-Dong Zhang(张雪东)¹, Fu-Qiang Zhang(张富强)², and Timothy C Steimle³

1 School of Physics and Information Engineering, Key Laboratory of Spectral Measurement and Analysis of Shanxi Province, Shanxi Normal University, Linfen 041004, China;
2 School of Chemical and Material Science, Key Laboratory of Magnetic Molecules & Magnetic Information Materials of Ministry of Education, Shanxi Normal University, Linfen 041004, China;
3 School of Molecular Science, Arizona State University, Tempe 85287, USA

收稿日期:2021-09-19 修回日期:2021-12-07 发布日期:2022-04-29
通讯作者: Xi-Lin Bai,E-mail:bxl5630@mail.ustc.edu.cn E-mail:bxl5630@mail.ustc.edu.cn
基金资助:
Project supported by the National Natural Science Foundation of China (Grant No.21903050).

Laser-induced fluorescence experimental spectroscopy and theoretical calculations of uranium monoxide

Xi-Lin Bai(白西林)^1,†, Xue-Dong Zhang(张雪东)¹, Fu-Qiang Zhang(张富强)², and Timothy C Steimle³

1 School of Physics and Information Engineering, Key Laboratory of Spectral Measurement and Analysis of Shanxi Province, Shanxi Normal University, Linfen 041004, China;
2 School of Chemical and Material Science, Key Laboratory of Magnetic Molecules & Magnetic Information Materials of Ministry of Education, Shanxi Normal University, Linfen 041004, China;
3 School of Molecular Science, Arizona State University, Tempe 85287, USA

Received:2021-09-19 Revised:2021-12-07 Published:2022-04-29
Contact: Xi-Lin Bai,E-mail:bxl5630@mail.ustc.edu.cn E-mail:bxl5630@mail.ustc.edu.cn
About author:2021-12-16
Supported by:
Project supported by the National Natural Science Foundation of China (Grant No.21903050).

摘要/Abstract

摘要： As a model molecule of actinide chemistry, UO molecule plays an important role in understanding the electronic structure and chemical bonding of actinide-containing species. We report a study of the laser-induced fluorescence spectra of the U¹⁶O and U¹⁸O using two-dimensional spectroscopy. Several rotationally resolved excitation spectra were investigated. Accurate molecular rotational constants and equilibrium internuclear distances were reported. Low-lying electronic states information was extracted from high resolution dispersed fluorescence spectra and analyzed by the ligand field theory model. The configuration of the ground state was determined as U²⁺(5f³7s)O^2-. The branching ratios, and the vibrational harmonic and anharmonic parameters were also obtained. Radiative lifetimes were determined by recording the time-resolved fluorescence spectroscopy. Transition dipole moments were calculated using the branching ratios and the radiative lifetimes. These findings were elucidated by using quantum-chemical calculations, and the chemical bonding was also analyzed. The findings presented in this work will enrich our understanding of actinide-containing molecules.

关键词: laser-induced fluorescence, two-dimensional spectroscopy, density functional theory

Abstract: As a model molecule of actinide chemistry, UO molecule plays an important role in understanding the electronic structure and chemical bonding of actinide-containing species. We report a study of the laser-induced fluorescence spectra of the U¹⁶O and U¹⁸O using two-dimensional spectroscopy. Several rotationally resolved excitation spectra were investigated. Accurate molecular rotational constants and equilibrium internuclear distances were reported. Low-lying electronic states information was extracted from high resolution dispersed fluorescence spectra and analyzed by the ligand field theory model. The configuration of the ground state was determined as U²⁺(5f³7s)O^2-. The branching ratios, and the vibrational harmonic and anharmonic parameters were also obtained. Radiative lifetimes were determined by recording the time-resolved fluorescence spectroscopy. Transition dipole moments were calculated using the branching ratios and the radiative lifetimes. These findings were elucidated by using quantum-chemical calculations, and the chemical bonding was also analyzed. The findings presented in this work will enrich our understanding of actinide-containing molecules.

Key words: laser-induced fluorescence, two-dimensional spectroscopy, density functional theory

中图分类号: (Molecular spectra)

33.20.-t

31.15.ae (Electronic structure and bonding characteristics) 42.62.Fi (Laser spectroscopy)

Xi-Lin Bai(白西林), Xue-Dong Zhang(张雪东), Fu-Qiang Zhang(张富强), and Timothy C Steimle. Laser-induced fluorescence experimental spectroscopy and theoretical calculations of uranium monoxide[J]. 中国物理B, 2022, 31(5): 53301-053301.

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Laser-induced fluorescence experimental spectroscopy and theoretical calculations of uranium monoxide

Laser-induced fluorescence experimental spectroscopy and theoretical calculations of uranium monoxide

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