Raman spectroscopic investigations were carried out on proposed nuclear fuel thorium dioxide-uranium dioxide (ThO<sub>2</sub>-UO<sub>2</sub>) solid solutions and simulated fuels based on ThO<sub>2</sub>-UO<sub>2</sub>. Raman spectra of ThO<sub>2</sub>-UO<sub>2</sub> solid solutions exhibited two-mode behavior in the entire composition range. Variations in mode frequencies and relative intensities of Raman modes enabled estimation of composition, defects, and oxygen stoichiometry in these compounds that are essential for their application. The present study shows that Raman spectroscopy is a simple, promising analytical tool for nondestructive characterization of this important class of nuclear fuel materials.

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