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Covalent dependence of octahedral rotations in orthorhombic perovskite oxides
Journal article   Peer reviewed

Covalent dependence of octahedral rotations in orthorhombic perovskite oxides

Antonio Cammarata and James M. Rondinelli
The Journal of chemical physics, v 141(11), pp 114704-114704
21 Sep 2014
PMID: 25240365

Abstract

Chemistry Chemistry, Physical Physical Sciences Physics Physics, Atomic, Molecular & Chemical Science & Technology
The compositional dependence of metal-oxygen BO6 octahedral distortions, including bond elongations and rotations, is frequently discussed in the ABO(3) perovskite literature; structural distortions alleviate internal stresses driven by under-or over-coordinated bond environments. Here we identify the dependence of octahedral rotations from changes in metal-oxygen bond covalency in orthorhombic perovskites. Using density functional theory we formulate a covalency metric, which captures both the real and k-space interactions between the magnitude and sense, i.e., in-phase or out-of-phase, octahedral rotations, to explore the link between the ionic-covalent Fe-O bond and the interoctahedral Fe-O-Fe bond angles in Pbnm ferrates. Our survey finds that the covalency of the metal-oxygen bond is correlated with the rotation amplitude: We find the more covalent the Fe-O bond, the less distorted is the structure and the more important the long-range inter-octahedral (Fe-O-Fe bond angle) interactions. Finally, we show how to indirectly tune the B-O bond covalency by A-cation induced BO6 rotations independent of ionic size, facilitating design of targeted bonding interactions in complex perovskites. (C) 2014 AIP Publishing LLC.

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Chemistry, Physical
Physics, Atomic, Molecular & Chemical
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