Atomistic Modeling of the Negative Thermal Expansion in δ- Plutonium Based on the Two-State Description
Abstract
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 et al. 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.
- Authors:
-
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. of California, San Diego, CA (United States). Jacobs School of Engineering
- Publication Date:
- Research Org.:
- Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division
- OSTI Identifier:
- 1628433
- Grant/Contract Number:
- AC52-06NA25396
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Materials
- Additional Journal Information:
- Journal Volume: 5; Journal Issue: 12; Journal ID: ISSN 1996-1944
- Publisher:
- MDPI
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; Materials Science; plutonium; negative thermal expansion; Invar; Weiss model; modified embedded atom method; Monte Carlo method
Citation Formats
Lee, Tongsik, Baskes, Michael I., Lawson, A. C., Chen, Shao Ping, and Valone, Steven M. Atomistic Modeling of the Negative Thermal Expansion in δ- Plutonium Based on the Two-State Description. United States: N. p., 2012.
Web. doi:10.3390/ma5061040.
Lee, Tongsik, Baskes, Michael I., Lawson, A. C., Chen, Shao Ping, & Valone, Steven M. Atomistic Modeling of the Negative Thermal Expansion in δ- Plutonium Based on the Two-State Description. United States. https://doi.org/10.3390/ma5061040
Lee, Tongsik, Baskes, Michael I., Lawson, A. C., Chen, Shao Ping, and Valone, Steven M. Thu .
"Atomistic Modeling of the Negative Thermal Expansion in δ- Plutonium Based on the Two-State Description". United States. https://doi.org/10.3390/ma5061040. https://www.osti.gov/servlets/purl/1628433.
@article{osti_1628433,
title = {Atomistic Modeling of the Negative Thermal Expansion in δ- Plutonium Based on the Two-State Description},
author = {Lee, Tongsik and Baskes, Michael I. and Lawson, A. C. and Chen, Shao Ping and Valone, Steven M.},
abstractNote = {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 et al. 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.},
doi = {10.3390/ma5061040},
journal = {Materials},
number = 12,
volume = 5,
place = {United States},
year = {Thu Jun 07 00:00:00 EDT 2012},
month = {Thu Jun 07 00:00:00 EDT 2012}
}
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