An approach to study the diffusion of plutonium (Pu) waste into the material of the storage containers is presented. The delta phase of Pu has been examined, in this article, using a spin and orbitally polarized ab-initio (full potential LMTO) approach [1, 2]. These computations are relatively inexpensive, and it is the intention to see if the results obtained would be satisfactory (compared to the accurate SIC-LDA computations [1-2]) for diffusive studies of Pu into the material of storage containers (for example, into FCC iron as a surrogate for steel ). The combination of LDA and spin and orbitally polarized LMTO calculations that we use successfully predict a delocalized 5f, (i.e. bonding) monoclinic ground state and a localized FCC excited state with a density about 8% greater than experiment (compared to the 30% error from pure LDA calculations by various groups [3-6]). The density of states is computed and compared to experimental photoemission studies; there is qualitative agreement. The spin, orbital and total magnetic moment for the FCC phase is computed; the results are qualitatively in agreement with those of other studies. An analytical method for studying the time-dependent diffusion of Pu across an interface with another atomic species is presented.
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Thanks to Dr. B. R. Cooper for providing an introduction to the electronic structure part of this work.
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Setty, A.K. Ab-initio Based Diffusive Studies of Plutonium with Relevance to Nuclear Waste Management. MRS Online Proceedings Library 824, 408–413 (2004). https://doi.org/10.1557/PROC-824-CC8.30