Artificial ferroelectric-like hysteresis in antiferroelectrics with non-uniform disorder

Abstract: Antiferroelectrics exhibit unique double-hysteresis polarization loops, which have garnered significant attention due to their potential applications such as energy storage, electromechanical transduction, as well as synapse devices. However, numerous antiferroelectric materials have been reported to display signs of hysteresis loops resembling those of ferroelectric materials, and a comprehensive understanding remains elusive. In this work, we provide a phenomenological model that reproduces such widely observed artificial ferroelectric hysteresis with a superposition of numerous disordered antiferroelectric loops that have varying antiferroelectric-to-ferroelectric transition fields, particularly when these field ranges intersect. Experimentally, we realized such artificial ferroelectric-like hysteresis loops in the prototypical antiferroelectric PbZrO$_3$ and PbHfO$_3$ thin films, by introducing non-uniform local disorder (e.g., defects) via fine-tuning of the film growth conditions. These ferroelectric-like states are capable of persisting for several hours prior to transitioning back into the thermodynamically stable antiferroelectric ground state. Those results provide insights into the fundamental impact of disorder on the AFE properties and new possibilities of disorder-tailored functions.