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The electric field-temperature phase diagrams for (Bi1/2Na1/2)TiO3-BaTiO3-(K1/2Na1/2)NbO3 relaxor ceramics

Abstract

The electric field-temperature (E-T) phase diagrams for three model compositions in the lead-free (Bi1/2Na1/2)TiO3-BaTiO3-(K1/2Na1/2)NbO3 (BNT-BT-KNN) relaxor system have been constructed, to serve as a template for other similar systems. The compositions chosen are known to exhibit non-ergodic (BNT-6BT), ergodic (BNT-6BT-3KNN) and ferroelectric (BNT-12BT) behavior at room temperature. Through temperature-dependent permittivity and piezoelectric measurements, the transition pathways across relaxor-ferroelectric states were determined as a function of temperature and electric field. The relaxor compositions were found to have a typical U-shaped E-T phase diagram and exhibited typical transitions to ferroelectric phase on applying electric field above threshold values. BNT-6BT is suggested to have a freezing temperature (Tf) of approximately 120 °C and exhibited a “mixed” transition behavior between 90 °C to 120 °C, characterized by a presence of both partially pinched polarization hysteresis loops, characteristic of ergodic relaxors, and substantial negative strains, indicating non-ergodic behavior. Similar behavior was observed for BNT-6BT-3KNN, which had a rather broad temperature range (21 °C to -40 °C) where it exhibited the “mixed” transition behavior. The field required for relaxor to ferroelectric transition was 20 kV/cm and 30 kV/cm for BNT-6BT and BNT-6BT-3KNN at Tf, respectively. BNT-12BT was ferroelectric at room temperature, however it transformed spontaneously to an ergodic relaxor at approximately 200 °C on heating. Additionally, to study the influence of point defects on the E-T phase diagrams, non-stoichiometry was intentionally introduced to alter oxygen vacancy concentration in the BNT-6BT composition. It was found that lowering the oxygen vacancy concentration lowers the Tf, while increasing their concentration has the opposite effect. This provides an avenue to tune crucial materials parameters such as Tf and critical field values and modify their structural transition pathways to suit application requirements.

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Publication details

The article was received on 22 Aug 2018, accepted on 25 Sep 2018 and first published on 28 Sep 2018


Article type: Paper
DOI: 10.1039/C8TC04189J
Citation: J. Mater. Chem. C, 2018, Accepted Manuscript
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    The electric field-temperature phase diagrams for (Bi1/2Na1/2)TiO3-BaTiO3-(K1/2Na1/2)NbO3 relaxor ceramics

    X. shi, N. Kumar and M. Hoffman, J. Mater. Chem. C, 2018, Accepted Manuscript , DOI: 10.1039/C8TC04189J

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