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Title: Thermal transport properties of halide solid solutions: Experiments vs equilibrium molecular dynamics

The composition dependence of thermal transport properties of the (Na,K)Cl rocksalt solid solution is investigated through equilibrium molecular dynamics (EMD) simulations in the entire range of composition and the results are compared with experiments published in recent work [Gheribi et al., J. Chem. phys. 141, 104508 (2014)]. The thermal diffusivity of the (Na,K)Cl solid solution has been measured from 473 K to 823 K using the laser flash technique, and the thermal conductivity was deduced from critically assessed data of heat capacity and density. The thermal conductivity was also predicted at 900 K in the entire range of composition by a series of EMD simulations in both NPT and NVT statistical ensembles using the Green-Kubo theory. The aim of the present paper is to provide an objective analysis of the capability of EMD simulations in predicting the composition dependence of the thermal transport properties of halide solid solutions. According to the Klemens-Callaway [P. G. Klemens, Phys. Rev. 119, 507 (1960) and J. Callaway and H. C. von Bayer, Phys. Rev. 120, 1149 (1960)] theory, the thermal conductivity degradation of the solid solution is explained by mass and strain field fluctuations upon the phonon scattering cross section. A rigorous analysis ofmore » the consistency between the theoretical approach and the EMD simulations is discussed in detail.« less
Authors:
;  [1] ;  [2]
  1. CRCT—Centre for Research in Computational Thermochemistry, Department of Chemical Engineering,École Polytechnique, P.O. Box 6079, Station Downtown, Montréal, Québec H3C 3A7 (Canada)
  2. Sorbonne Universits, UPMC Univ Paris 06, UMR 8234, PHENIX, F-75005 Paris (France)
Publication Date:
OSTI Identifier:
22415554
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 142; Journal Issue: 12; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; COMPARATIVE EVALUATIONS; CROSS SECTIONS; DENSITY; EQUILIBRIUM; FLUCTUATIONS; KUBO FORMULA; MOLECULAR DYNAMICS METHOD; PHONONS; POTASSIUM CHLORIDES; SODIUM CHLORIDES; SOLID SOLUTIONS; SPECIFIC HEAT; STRAINS; TEMPERATURE DEPENDENCE; THERMAL CONDUCTIVITY; THERMAL DIFFUSIVITY