Modeling oxygen diffusion in barium titanate using molecular dynamics: Comparison between Mg and Sc dopants
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In: The journal of physics and chemistry of solids : JPCS, Vol. 181.2023, No. October, 111525, 27.06.2023.
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TY - JOUR
T1 - Modeling oxygen diffusion in barium titanate using molecular dynamics
T2 - Comparison between Mg and Sc dopants
AU - Preis, Wolfgang
N1 - Publisher Copyright: © 2023 Elsevier Ltd
PY - 2023/6/27
Y1 - 2023/6/27
N2 - In this study, the diffusion coefficient of oxygen vacancies in barium titanate doped with 2.0% Sc was calculated by using molecular dynamics. The temperature was varied from 1273 K to 2500 K, and the simulation box consisted of 10 × 10 × 10 unit cells subject to periodic boundary conditions. The Sc dopants were incorporated into the B-sublattice and compensated for by using the randomly distributed oxygen vacancies on the oxygen sublattice. The diffusivity of the vacancies was determined from the slope of the mean-squared displacement of the oxygen ions over time. The Arrhenius plot of the diffusion coefficient showed a clear linear behavior, with an activation energy of 0.84 eV. The results were interpreted by computing radial pair distribution functions for various correlations (e.g., Ti–O and Sc–O) and by static lattice (nudged elastic band) calculations of energy barriers for the migration of oxygen. While Mg-doped BaTiO 3 exhibited a strong trend of the formation of defect associates between the acceptor dopant and the oxygen vacancies that lead to a clear reduction in the observed activation energy for oxygen transport with increasing temperature (non-linear Arrhenius behavior), defect-induced interactions (associates) in case of Sc doping were nearly negligibly small, and gave rise to a linear Arrhenius plot with a single activation energy.
AB - In this study, the diffusion coefficient of oxygen vacancies in barium titanate doped with 2.0% Sc was calculated by using molecular dynamics. The temperature was varied from 1273 K to 2500 K, and the simulation box consisted of 10 × 10 × 10 unit cells subject to periodic boundary conditions. The Sc dopants were incorporated into the B-sublattice and compensated for by using the randomly distributed oxygen vacancies on the oxygen sublattice. The diffusivity of the vacancies was determined from the slope of the mean-squared displacement of the oxygen ions over time. The Arrhenius plot of the diffusion coefficient showed a clear linear behavior, with an activation energy of 0.84 eV. The results were interpreted by computing radial pair distribution functions for various correlations (e.g., Ti–O and Sc–O) and by static lattice (nudged elastic band) calculations of energy barriers for the migration of oxygen. While Mg-doped BaTiO 3 exhibited a strong trend of the formation of defect associates between the acceptor dopant and the oxygen vacancies that lead to a clear reduction in the observed activation energy for oxygen transport with increasing temperature (non-linear Arrhenius behavior), defect-induced interactions (associates) in case of Sc doping were nearly negligibly small, and gave rise to a linear Arrhenius plot with a single activation energy.
KW - Acceptor doping
KW - Barium titanate
KW - Defect-induced interactions
KW - Diffusion of oxygen vacancies
KW - Molecular dynamics
UR - http://www.scopus.com/inward/record.url?scp=85162835154&partnerID=8YFLogxK
U2 - 10.1016/j.jpcs.2023.111525
DO - 10.1016/j.jpcs.2023.111525
M3 - Article
VL - 181.2023
JO - The journal of physics and chemistry of solids : JPCS
JF - The journal of physics and chemistry of solids : JPCS
SN - 0022-3697
IS - October
M1 - 111525
ER -