Ab initio molecular dynamics simulations of negative thermal expansion in ScF3: The effect of the supercell size

被引：20

作者：

Bocharov, D. ^{[1
]}

Krack, M. ^{[2
]}

Rafalskij, Yu ^{[1
]}

Kuzmin, A. ^{[1
]}

Purans, J. ^{[1
]}

机构：

[1] Univ Latvia, Inst Solid State Phys, Kengaraga St 8, LV-1063 Riga, Latvia

[2] Paul Scherrer Inst, Forschungsstr 111, CH-5232 Villigen, Switzerland

来源：

COMPUTATIONAL MATERIALS SCIENCE | 2020年 / 171卷

关键词：

ScF3; Negative thermal expansion; Ab initio molecular dynamics; EXAFS; CP2K; RIGID UNIT MODES; PHASE-TRANSITIONS; PSEUDOPOTENTIALS;

D O I：

10.1016/j.commatsci.2019.109198

中图分类号：

T [工业技术];

学科分类号：

08 ;

摘要：

Scandium fluoride (ScF3) belongs to a class of negative thermal expansion (NTE) materials. It shows a strong lattice contraction up to about 1000 K switching to expansion at higher temperatures. Here the NTE effect in ScF3 is studied in the temperature range from 300 K to 1600 K using ab initio molecular dynamics (AIMD) simulations in the isothermal-isobaric (NpT) ensemble. The temperature dependence of the lattice constant, inter-atomic Sc-F-Sc bond angle distributions and the Sc-F and Sc-Sc radial distribution functions is obtained as a function of supercell size from 2a x 2a x 2a to 5a x 5a x 5a where a is the lattice parameter of ScF3. A comparison with the experimental Sc K-edge EXAFS data at 600 K is used to validate the accuracy of the AIMD simulations. Our results suggest that the AIMD calculations are able to reproduce qualitatively the NTE effect in ScF3, however a supercell size larger than 2a x 2a x 2a should be used to account accurately for dynamic disorder. The origin of the NTE in ScF3 is explained by the interplay between expansion and rotation of ScF6 octahedra.

引用

页数：7

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