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Influence of a co-substituted A-site on structural characteristics and ferroelectricity of (Pb, Ba, Ca)TiO3 complex perovskites: analysis of local-, medium- and long-range order

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Abstract

Thin films of A-site co-substituted, PbTiO3 (PTO) by Ba2+ and Ca2+, i.e., PBCT70, PBCT60, PBCT50 and PBCT40 were fabricated on Pt/Ti/SiO2/Si substrates by chemical solution deposition. Structures of the samples were investigated from the viewpoint of local-, medium- and long-range order by X-ray absorption near structure (XANES), micro-Raman and infrared spectroscopies and by X-ray diffraction (XRD). The films thickness were determined by using field-emission scanning electron microscope. The experimental results demonstrate that BaO12 clusters are the critical dominant ferroelectricity cause in PBCT thin films rather than CaO12 clusters. XRD analysis which was applied to investigate the crystal symmetry indicates the absence of long-range structural distortion for samples at higher concentrations of Ba2+ and Ca2+. However, an analysis of structural medium- and local-range order such as infrared, micro-Raman and XANES spectroscopies revealed that symmetry changes are much more prominent; i.e., local structural distortions remain. Temperature-dependent dielectric permittivity measurements confirmed a decreasing ferroelectric-to-paraelectric phase transition temperature and showed a broad phase transition with an increase in BaO12 and CaO12 clusters. In addition, the lack of long-range polar ordering for the ferroelectric dipole caused by symmetry changes decreases the remanent polarization.

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Acknowledgments

This work was financially supported by the Brazilian agencies FAPESP, CNPq and CAPES. We thank CEPID/CMDMC/INCTMN/CDMF. FAPESP process nos. 08/57150-6 and 11/20536-7. This research was partially performed at LNLS, Campinas, SP, Brazil.

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Authors and Affiliations

  1. LIEC, Department of Chemistry, Universidade Federal de São Carlos, Via Washington Luiz, km 235, P. O. Box 676, São Carlos, São Paulo, 13565-905, Brazil

    D. S. L. Pontes & E. Longo

  2. Department of Chemistry, Universidade Estadual Paulista (UNESP), P. O. Box 473, Bauru, São Paulo, 17033-360, Brazil

    F. M. Pontes

  3. Institute of Physics of São Carlos, USP, São Carlos, São Paulo, 13560-250, Brazil

    L. F. da Silva

  4. NanO LaB, Department of Physics, Universidade Federal de São Carlos, Via Washington Luiz, km 235, P. O. Box 676, São Carlos, São Paulo, 13565-905, Brazil

    A. J. Chiquito

  5. Department of Physics, UFSCar, Via Washington Luiz, km 235, São Carlos, São Paulo, CEP 13565-905, Brazil

    P. S. Pizani

  6. Institute of Chemistry, Universidade Estadual Paulista (UNESP), Araraquara, São Paulo, Brazil

    E. Longo

Authors
  1. D. S. L. Pontes
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  2. F. M. Pontes
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  3. L. F. da Silva
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  4. A. J. Chiquito
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  5. P. S. Pizani
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  6. E. Longo
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Correspondence to F. M. Pontes.

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Pontes, D.S.L., Pontes, F.M., da Silva, L.F. et al. Influence of a co-substituted A-site on structural characteristics and ferroelectricity of (Pb, Ba, Ca)TiO3 complex perovskites: analysis of local-, medium- and long-range order. J Sol-Gel Sci Technol 69, 605–616 (2014). https://doi.org/10.1007/s10971-014-3265-0

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  • DOI: https://doi.org/10.1007/s10971-014-3265-0

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