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Parameterizing empirical interatomic potentials for predicting thermophysical properties via an irreducible derivative approach: the case of ThO2 and UO2

Journal Article · · Journal of Physics: Condensed Matter
 [1];  [1];  [2];  [2];  [3];  [4];  [1];  [5];  [2]
  1. Idaho National Laboratory (INL), Idaho Falls, ID (United States)
  2. Columbia Univ., New York, NY (United States)
  3. Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
  4. Pennsylvania State Univ., University Park, PA (United States)
  5. The Ohio State Univ., Columbus, OH (United States)
+ Show Author Affiliations
The accuracy of classical physical property predictions using molecular dynamics simulations is determined by the quality of the interatomic potentials. Here we introduce a training approach for empirical interatomic potentials (EIPs) which is well suited for capturing phonons and phonon-related properties. Our approach is based on direct comparisons of the second- and third-order irreducible derivatives (IDs) between an EIP and the Born–Oppenheimer potential within density functional theory (DFT) calculations. IDs fully exploit space group symmetry and allow for training without redundant information. We demonstrate the fidelity of our approach in the context of ThO2 and UO2, where we optimize parameters of an embedded-atom method potential in addition to core–shell interactions. Our EIPs provide thermophysical properties in good agreement with DFT and outperform widely utilized EIPs for phonon dispersion and thermal conductivity predictions. Reasonable estimates of thermal expansion and formation energies of Frenkel pairs are also obtained.
Research Organization:
Idaho National Laboratory (INL), Idaho Falls, ID (United States)
Sponsoring Organization:
National Energy Research Scientific Computing Center (NERSC); USDOE Office of Nuclear Energy (NE); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
Grant/Contract Number:
AC02-05CH11231; AC07-05ID14517; SC0016507
OSTI ID:
2581111
Report Number(s):
INL/JOU--22-66665-Rev001
Journal Information:
Journal of Physics: Condensed Matter, Journal Name: Journal of Physics: Condensed Matter Journal Issue: 25 Vol. 37; ISSN 0953-8984; ISSN 1361-648X
Publisher:
IOP PublishingCopyright Statement
Country of Publication:
United States
Language:
English

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Assessment of empirical interatomic potential to predict thermal conductivity in ThO2 and UO2
Journal Article · Thu May 27 20:00:00 EDT 2021 · Journal of Physics. Condensed Matter · OSTI ID:1809936

Related Subjects

empirical interatomic potential
molecular dynamics
potential training
thermal transport
thorium dioxide
uranium dioxide