Crystal structural evolution and hybrid improper ferroelectricity in Ruddlesden-Popper Ca3-xSrxTi2O7 ceramics

Hybrid improper ferroelectricity (HIF) has been proposed as a candidate approach to create room-temperature multiferroic materials with an intrinsic electric-field controlled magnetism effect, and HIFs in bi-layered Ruddlesden-Popper Ca3-xSrxTi2O7 ceramics have been confirmed in the present work. The ferroelectric hysteresis loops are observed in these ceramics at room temperature, and the polar orthorhombic structures with oxygen octahedral rotation and tilt modes have been confirmed by room-temperature X-ray powder diffraction. The amplitudes of oxygen octahedral rotation and tilt modes decrease with the increasing x value, which in turn leads to the decrease of remnant polarization in these ceramics. A first-order phase transition has been evidenced by the differential scanning calorimetry measurement, and the temperature of phase transition decreases linearly with the increasing content of strontium cations. It is found that the amplitude of oxygen octahedral distortion is the dominating factor that affects ferroelectric polarization in partial-ordered bi-layered Ca3Ti2O7-based ceramics.