Journal
ACTA MATERIALIA
Volume 122, Issue -, Pages 266-276Publisher
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.actamat.2016.09.050
Keywords
Graded thin films; Ferroelectric; Dielectric constant; Semiconductor; Thermodynamics
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Functional materials with compositional gradients exhibit unique characteristics that are different from the components comprising the structure. Graded ferroelectrics are very good examples to such materials where a systematic variation in composition is introduced along the thickness of a thin film heterostructure. Such structures display interesting properties including the, disappearance of the dielectric anomaly at the ferroelectric-paraelectric transition that is otherwise observed in monolayer ferroelectrics, a strong internal (built-in) electric field, low dielectric loss, and an almost temperature insensitive dielectric tunability. We present here a theoretical study to understand some interesting properties of graded ferroelectrics by treating these as wide band gap semiconductors. Such an approach allows us to address the effect of impuritiesidopants. We specifically analyze compositionally graded (001) hetero-epitaxial (Pb,Sr)TiO3 films between Pt electrodes on (001) SrTiO3. Our analysis shows that a single domain state could be stabilized in the presence of space charges whereas intrinsic stacks display wedge-like electrical domain patterns. The computations also provide an explanation as to why graded ferroelectrics should have lower dielectric losses and lower leakage currents compared to monolayer ferroelectrics., We attribute this to the carrier depletion in the layers due to built-in electric fields resulting from the polarization mismatch. (C) 2016 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.
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