Abstract
The electronic and thermodynamic complexity of plutonium has resisted a fundamental understanding for this important elemental metal. A critical test of any theory is the unusual softening of the bulk modulus with increasing temperature, a result that is counterintuitive because no or very little change in the atomic volume is observed upon heating. This unexpected behavior has in the past been attributed to competing but never-observed electronic states with different bonding properties similar to the scenario with magnetic states in Invar alloys. Using the recent observation of plutonium dynamic magnetism, we construct a theory for plutonium that agrees with relevant measurements by using density-functional-theory (DFT) calculations with no free parameters to compute the effect of longitudinal spin fluctuations on the temperature dependence of the bulk moduli in δ-Pu. We show that the softening with temperature can be understood in terms of a continuous distribution of thermally activated spin fluctuations.
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