The complex structural mechanisms behind strain curves in bismuth sodium titanate–barium titanate

In this work, the lead-free composition (1-x)Bi0.5Na0.5TiO3–xBaTiO3 (BNT–BT) with x = 0.12 was investigated using in situ Synchrotron x-ray powder diffraction. With the applied electric field, the pseudo-cubic relaxor phase reversibly transforms to a ferroelectric state. The reversibility is still preserved after 104 bipolar electric field cycles. A Rietveld refinement with a structure, strain, and texture analysis using a model based on the atomic scale was applied for four frequencies from 10−4 to 101 Hz. The analysis allowed us to separately determine the two coexisting phases, their electric field dependent evolution, and the underlying strain mechanisms. For all the applied frequencies, we showed that domain switching is the only strain mechanism appearing in the tetragonal phase and the lattice strain is the only mechanism in the rhombohedral phase. The coercive field of the tetragonal phase (4 kV/mm) is found to be higher than that of the rhombohedral phase (3 kV/mm). This divergence has not been observed in previously investigated lead-containing materials and cannot be detected solely using macroscopic strain and polarization experiments. Moreover, the domain strain abruptly starts to occur only after a threshold field value and exhibits high hysteresis. The lattice strain, on the other hand, starts nearly from the beginning and increases more linearly during the bipolar field cycle. It could, therefore, be demonstrated that complex structural mechanisms underlie the apparent clear and continuous macroscopic strain curve. These findings are crucial for all actuator materials undergoing a relaxor to ferroelectric phase transformation and provide approaches and strategies to optimize lead-free materials for tailored applications.