The impact of chemical order on defect transport in mixed pyrochlores

Literature Information

Publication Date 2019-02-19
DOI 10.1039/C8CP07597B
Impact Factor 3.676
Authors

Blas P. Uberuaga, Romain Perriot, Ghanshyam Pilania


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Abstract

Using temperature accelerated dynamics, an accelerated molecular dynamics method, we examine the relationship between composition and cation ordering and defect transport in the mixed pyrochlore Gd2(Ti1−xZrx)2O7, using the oxygen vacancy as a representative defect structure. We find that the nature of transport is very sensitive to the cation structure, transitioning, as a function of composition, from three-dimensional migration to two-dimensional to pseudo-one-dimensional to becoming essentially immobile before reverting back to three-dimensional as the Zr content is increased. The rates of migration are also affected by the cation structure in the various compositions. This behavior is driven by the connectivity of Ti polyhedra in the material, with more extensive networks of Ti ions leading to a greater ability of the vacancy to traverse the material. Our results indicate that the nature of transport is dictated by the cation structure of the material and that, conversely, the cation structure could be used to control transport and potentially other functionalities in mixed pyrochlores.

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Source Journal

Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
Self-citation Rate: 10.3%
Articles per Year: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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