Optical properties and electronic structure of UO2

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Abstract
The near normal incidence reflectivity of UO2 single crystals has been measured in the photon energy range from 0.03 eV to 13 eV. From the reflectivity spectrum the complex dielectric function ε (ω) =ε1(ω)+iε2(ω) has been derived by means of the Kramers-Kronig relation. In addition the absorption coefficient was determined from a direct transmission measurement on thin single crystal plates in the weakly absorbing spectral region below the absorption edge. An energy level scheme is proposed which allows a self-consistent assignment of the structure in ε2 with optical transitions between maxima in the density of states. The energy gap found at 2.1±0.1 eV is attributed to a 5f2→5f16deg transition. A crystal field splitting 10Dq=2.8 eV is derived for the 6d conduction states. Good agreement is obtained within this model with XPS measurements and a recent molecular cluster approximation. It disagrees with a previous interpretation of reflectivity data.

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