Quantifying the Importance of Orbital Over Spin Correlations in δ-Pu Within Density-Functional Theory

Abstract

The electronic structure of plutonium is studied within the density-functional theory (DFT) model. Key features of the electronic structure are correctly modeled and bonding, total energy, and electron density of states are all consistent with measure data, although the prediction of magnetism is not consistent with many observations. Here we analyze the contributions to the electronic structure arising from spin polarization, orbital polarization, and spin-orbit interaction. These effects give rise to spin and orbital moments that are of nearly equal magnitude, but anti-parallel, suggesting a magnetic-moment cancellation with a zero total moment. Quantifying the spin versus orbital effects on the bonding, total energy, and electron spectra it becomes clear that the spin polarization is much less important than the orbital correlations. Consequently, a restricted DFT approach with a non-spin polarized electronic structure can produce reasonable equation-of-state and electron spectra for δ-Pu when the orbital effects are accounted for. Hence, we present two non-magnetic models. One in which the spin moment is canceled by the orbital moment and another in which the spin moment (and therefore the orbital moment) is restricted to zero.

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Correspondence to Per Soderlind.

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Soderlind, P. Quantifying the Importance of Orbital Over Spin Correlations in δ-Pu Within Density-Functional Theory. MRS Online Proceedings Library 1104, 203 (2008). https://doi.org/10.1557/PROC-1104-NN02-03

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