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Electronic spectroscopy of UO(2)Cl(2) isolated in solid Ar.

Jin Jin¹, Raj Gondalia, Michael C Heaven

¹Department of Chemistry, Emory University, Atlanta, Georgia 30322, USA.

The Journal of Physical Chemistry. A

|July 28, 2009

Summary

Researchers studied uranyl chloride in argon using laser-induced fluorescence. They observed distinct absorption and emission spectra, confirming transitions within the uranyl ion (UO2+2) subunit.

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Area of Science:

Spectroscopy
Inorganic Chemistry
Quantum Chemistry

Background:

Uranyl compounds are important in nuclear energy and environmental science.
Understanding their electronic structure is crucial for predicting chemical behavior.
Solid-state matrix isolation provides a controlled environment for studying molecular properties.

Purpose of the Study:

To investigate the electronic and vibrational properties of uranyl chloride (UO2Cl2) in a solid argon matrix.
To characterize the absorption and emission spectra of UO2Cl2 under pulsed laser excitation.
To correlate experimental observations with theoretical calculations for electronic transitions.

Main Methods:

Laser-induced fluorescence (LIF) spectroscopy.
Pulsed excitation using XeCl excimer laser (308 nm) and a tunable dye laser (19500–27500 cm-1).
Isolation of uranyl chloride in a solid argon (Ar) matrix at low temperatures.

Main Results:

Observed distinct absorption and emission band systems for UO2Cl2 in Ar.
Emission spectra showed a harmonic vibrational progression (840 cm-1) originating at 20323 cm-1.
Absorption spectra featured five harmonic vibrational progressions (~710 cm-1).
Transitions were assigned to the UO2+2 subunit, involving electron promotion to 5f orbitals.
Fluorescence originated solely from the lowest-energy excited state.
Biexponential decay with lifetimes of 50 and 260 microseconds was measured.

Conclusions:

The study successfully characterized the spectroscopic properties of uranyl chloride in a solid argon matrix.
Experimental results align with theoretical predictions regarding electronic transitions within the UO2+2 moiety.
The observed fluorescence and decay kinetics provide insights into the excited-state dynamics of uranyl chloride.