Atomistic Modeling of the Negative Thermal Expansion in δ- Plutonium  Based on the Two-State Description

oleh: Steven M. Valone, A. C. Lawson, Shao Ping Chen, Tongsik Lee, Michael I. Baskes

Format: Article
Diterbitkan: MDPI AG 2012-06-01

Deskripsi

The δ phase  of plutonium with the fcc structure exhibits an unusual negative thermal expansion (NTE) over its narrow  temperature range of stability, 593–736 K. An accurate description  of the anomalous high-temperature volume effect of plutonium  goes beyond the current capability  of electronic-structure  calculations.  We propose an atomistic scheme to model the thermodynamic properties of δ-Pu based on the two-state model of Weiss for the Invar alloys, inspired by the simple free-energy analysis previously conducted by Lawson<em> et al.</em> The two-state mechanism is incorporated into the atomistic description of a many-body  interacting  system.  Two modified  embedded atom method potentials are employed to represent the binding energies of two competing  electronic  states in δ-Pu. We demonstrate how the NTE takes place in δ-Pu by means of Monte Carlo simulations implemented with the two-state mechanism.