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Property engineering in BaTiO3 films by stoichiometry control

Published online by Cambridge University Press:  31 January 2011

J.F. Ihlefeld*
Affiliation:
Department of Materials Science and Engineering, North Carolina State University, Raleigh, North Carolina 27606; and Materials Science and Engineering Center, Sandia National Laboratories, Albuquerque, New Mexico 87185
S.M. Aygün
Affiliation:
Department of Materials Science and Engineering, North Carolina State University, Raleigh, North Carolina 27606
W.J. Borland
Affiliation:
Dupont Electronic Technologies, Research Triangle Park, North Carolina 27709
J-P. Maria*
Affiliation:
Department of Materials Science and Engineering, North Carolina State University, Raleigh, North Carolina 27606
*
a)Address all correspondence to this author. e-mail: jihlefe@sandia.gov
b)Address all correspondence to this author. e-mail: jpmaria@ncsu.edu
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Abstract

BaTiO3 thin films were prepared on metallic foil substrates using chemical solution deposition. The impact of A to B site cation ratios on the phase assemblage and microstructural and dielectric properties was investigated by characterizing a sample set that includes stoichiometric BaTiO3 and 1, 2, 3, 4, and 5 mol% excess BaO. Each composition was subjected to a high-temperature anneal step with maximum dwell temperatures of 1000, 1100, and 1200 °C for 20 h. Excess barium concentrations greater than 3% lead to dramatic grain growth and average grain sizes exceeding 1 μm. Despite the large deviations from stoichiometry and the 20 h dwell time at temperature, x-ray diffraction, and high-resolution electron microscopy analysis were unable to detect secondary phases until films with 5% excess barium were annealed to 1200 °C. Thin films with 3% excess barium were prepared on copper substrates and annealed at 1060 °C, the practical limit for copper. This combination of BaO excess and annealing temperature produced an average lateral grain size of 0.8 μm and a room-temperature permittivity of 4000. This is in comparison to a permittivity of 1800 for stoichiometric material prepared using identical conditions. This work suggests metastable solubility of BaO in BaTiO3 that leads to enhanced grain growth and large permittivity values. This technique provides a new solid-state means of achieving grain growth in low thermal budget systems.

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Articles
Copyright
Copyright © Materials Research Society 2010

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