Abstract
The occupationally disordered structures and associated local polar fluctuations in lead-free relaxors determine their electrical properties that are also sensitive to external stimuli. These stimuli can lead to phase transitions, and the associated enhancement in the electro-mechanical responses necessitate a better understanding of these transitions. Here we report a non-canonical spontaneous phase transition from a relaxor to a ferroelectric phase in (Na1/2Bi1/2)TiO3-BaTiO3 with temperature. With the help of experiments (dielectric permittivity, diffraction, differential scanning calorimetry, polarization and Raman spectroscopy), a complete picture of the temperature evolution of relaxor behavior leading to this spontaneous phase transition has been reported. Furthermore, it has been shown that internal chemical pressure from oxygen vacancies can be utilized to tailor these phase transitions. Finally, an electric field-temperature phase diagram has been proposed with an emphasis on the influence of the defect chemistry. This work provides new insights into the origin of these spontaneous phase transitions.
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