Effect of acceptor dopants on the proton mobility in BaZr O3

A density functional investigation

Mårten E. Björketun, Per G. Sundell, Göran Wahnström

Resultado de la investigación: Article

97 Citas (Scopus)

Resumen

In this work, the stability and mobility of protonic defects in acceptor doped BaZr O3 are investigated using density functional theory in conjunction with kinetic modeling. The interaction between the mobile protons and Zr-site substituted trivalent dopants-Ga, Sc, In, Y, and Gd-is assessed by extensive mapping of migration pathways. In all cases, the interaction is attractive, which results in a stabilization, and hence a reduction of the mobility, of the proton. However, its strength and range vary substantially and are found to be strongly correlated to the ionic radius of the dopant. Further, it is shown that the observed correlation is related to a variation in strength of hydrogen bonds formed between protons and next nearest lattice oxygen ions in different environments. Finally, migration barriers and attempt frequencies obtained from first principles are used as input to a jump-diffusion model. The proton self-diffusion coefficient is evaluated for the different substituted phases, and the experimental trend in activation energies is reproduced.

Idioma originalEnglish
Número de artículo054307
PublicaciónPhysical Review B - Condensed Matter and Materials Physics
Volumen76
N.º5
DOI
EstadoPublished - 23 ago 2007

Huella dactilar

Protons
Doping (additives)
protons
oxygen ions
Density functional theory
Hydrogen bonds
diffusion coefficient
Stabilization
Activation energy
stabilization
interactions
Ions
hydrogen bonds
Oxygen
activation energy
density functional theory
trends
Defects
Kinetics
radii

ASJC Scopus subject areas

  • Condensed Matter Physics
  • Electronic, Optical and Magnetic Materials

Citar esto

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abstract = "In this work, the stability and mobility of protonic defects in acceptor doped BaZr O3 are investigated using density functional theory in conjunction with kinetic modeling. The interaction between the mobile protons and Zr-site substituted trivalent dopants-Ga, Sc, In, Y, and Gd-is assessed by extensive mapping of migration pathways. In all cases, the interaction is attractive, which results in a stabilization, and hence a reduction of the mobility, of the proton. However, its strength and range vary substantially and are found to be strongly correlated to the ionic radius of the dopant. Further, it is shown that the observed correlation is related to a variation in strength of hydrogen bonds formed between protons and next nearest lattice oxygen ions in different environments. Finally, migration barriers and attempt frequencies obtained from first principles are used as input to a jump-diffusion model. The proton self-diffusion coefficient is evaluated for the different substituted phases, and the experimental trend in activation energies is reproduced.",
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Effect of acceptor dopants on the proton mobility in BaZr O3 : A density functional investigation. / Björketun, Mårten E.; Sundell, Per G.; Wahnström, Göran.

En: Physical Review B - Condensed Matter and Materials Physics, Vol. 76, N.º 5, 054307, 23.08.2007.

Resultado de la investigación: Article

TY - JOUR

T1 - Effect of acceptor dopants on the proton mobility in BaZr O3

T2 - A density functional investigation

AU - Björketun, Mårten E.

AU - Sundell, Per G.

AU - Wahnström, Göran

PY - 2007/8/23

Y1 - 2007/8/23

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AB - In this work, the stability and mobility of protonic defects in acceptor doped BaZr O3 are investigated using density functional theory in conjunction with kinetic modeling. The interaction between the mobile protons and Zr-site substituted trivalent dopants-Ga, Sc, In, Y, and Gd-is assessed by extensive mapping of migration pathways. In all cases, the interaction is attractive, which results in a stabilization, and hence a reduction of the mobility, of the proton. However, its strength and range vary substantially and are found to be strongly correlated to the ionic radius of the dopant. Further, it is shown that the observed correlation is related to a variation in strength of hydrogen bonds formed between protons and next nearest lattice oxygen ions in different environments. Finally, migration barriers and attempt frequencies obtained from first principles are used as input to a jump-diffusion model. The proton self-diffusion coefficient is evaluated for the different substituted phases, and the experimental trend in activation energies is reproduced.

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