Electronically driven collapse of the bulk modulus in $\delta$-plutonium

TL;DR

This paper explains the anomalous softening of plutonium's bulk modulus at high temperatures as due to the compressibility of thermally excited electronic states, challenging conventional models.

Contribution

It introduces the concept that electronic configuration compressibility causes bulk modulus softening, a factor previously overlooked in thermodynamic models of plutonium.

Findings

Electronic configurations' compressibility explains bulk modulus softening.

Softening occurs regardless of thermal expansion sign.

Results align with elastic measurements on gallium-stabilized δ-plutonium.

Abstract

Plutonium metal exhibits an anomalously large softening of its bulk modulus at elevated temperatures that is made all the more extraordinary by the finding that it occurs irrespective of whether the thermal expansion coefficient is positive, negative or zero --- representing an extreme departure from conventional Gr\"{u}neisen scaling. We show here that the cause of this softening is the compressibility of plutonium's thermally excited electronic configurations, which has thus far not been considered in thermodynamic models. We show that when compressible electronic configurations are thermally activated, they invariably give rise to a softening of bulk modulus regardless of the sign their contribution to the thermal expansion. The electronically driven softening of the bulk modulus is shown to be in good agreement with elastic moduli measurements performed on the gallium-stabilized $\delta$ phase of plutonium over a range of temperatures and compositions, and is shown to grow rapidly at small concentrations of gallium and at high temperatures, where it becomes extremely sensitive to hydrostatic pressure.