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Orbital Hybridization in Uranium Compounds and its Influence on Electronic Properties

Published online by Cambridge University Press:  01 February 2011

Wei Wang ,
Hong Zhang  and
Guokui Liu
Wei Wang
Affiliation:
[email protected], Argonne National Laboratory, Argonne, IL, 60439, United States
Hong Zhang
Affiliation:
[email protected], Argonne National Laboratory, Argonne, IL, 60439, United States
Guokui Liu
Affiliation:
[email protected], Argonne National Laboratory, Chemical Sciences and Engineering, B200, Argonne, IL, 60439, United States
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Abstract

Computational analysis and modeling of spectroscopic properties of trivalent uranium in crystals of hexagonal symmetry have been conducted with inclusion of the crystal-field induced orbital hybridization between the 5f3 and 5f26d configurations. It is shown that, in the absorption spectrum with energy above 20,000 cm-1, the mixing of 5f3 and 5f26d states is significant. The spectrum in this region cannot be interpreted by the conventional model of crystal field theory. The Judd-Ofelt theory is completely failed in predicating the intensities of optical absorption from the ground state to the configuration mixed excited states. A new Hamiltonian including the odd ranks of crystal field interaction is diagonalized on the bases of all 5f3 and 5f26d states. A simulation of absorption spectrum is optimized in comparison with the experimental spectrum for determination of the Hamiltonian parameters.

Keywords

electronic structureabsorptionoptical properties
Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 1104: Symposium NN – Actinides 2008—Basic Science, Applications and Technology , 2008 , 1104-NN04-08
Copyright
Copyright © Materials Research Society 2008

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