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The Origin of Electrical Activity at Grain Boundaries in Perovskites and Related Materials

Published online by Cambridge University Press:  21 March 2011

S. J. Pennycook ,
M. Kim ,
G. Duscher ,
N. D. Browning ,
K. Sohlberg  and
S. T. Pantelides
S. J. Pennycook
Affiliation:
Solid State Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831-6030 Department of Physics and Astronomy, Vanderbilt University, Nashville TN 37235
M. Kim
Affiliation:
Solid State Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831-6030 Department of Physics, University of Illinois at Chicago, Chicago, IL 60607-7059
G. Duscher
Affiliation:
Solid State Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831-6030 Department of Physics and Astronomy, Vanderbilt University, Nashville TN 37235
N. D. Browning
Affiliation:
Department of Physics, University of Illinois at Chicago, Chicago, IL 60607-7059
K. Sohlberg
Affiliation:
Department of Department of Chemistry, Drexel University, 3141 Chestnut Street, Philadelphia, PA 19104
S. T. Pantelides
Affiliation:
Solid State Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831-6030 Department of Physics and Astronomy, Vanderbilt University, Nashville TN 37235
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Extract

In the last few years, the combination of atomic-resolution Z-contrast microscopy, electron energy loss spectroscopy and first-principles theory has proved to be a powerful means for structure property correlations in complex materials1. Here we demonstrate the effectiveness of this combined approach by demonstrating the origins of electrical activity at grain boundaries in the prototypical perovskite SrTiO3 and the high-temperature superconductor YBa2Cu3O7-x, materials that are closely related in structure. We show, both experimentally and theoretically, that grain boundaries in SrTiO3 are intrinsically non-stoichiometric. Electron energy-loss spectroscopy (EELS) provides direct evidence of non-stoichiometry, in agreement with total- energy calculations that predict non-stoichiometric grain boundaries to be energetically favorable. The predicted structures are consistent with atomic-resolution Z-contrast micrographs. These results provide a consistent explanation of the grain boundary charge that was previously inferred from electrical measurements, and provides a microscopic explanation of the resulting “double-Schottky barriers”. We also present experimental evidence for non-stoichiometry at grain boundaries in the high-temperature superconductor YBa2Cu3O7-x, where the same phenomenon explains the observed exponential reduction of critical currents with grain boundary misorientation.

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 654: Symposia AA – Structure-Property Relationships of Oxide Surfaces & Interfaces , 2000 , AA1.3.1
Copyright
Copyright © Materials Research Society 2001

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