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

Yi Zhang#, Xinyu Zhang#, Zihao Zheng#, Jiyang Xie, Jing Lou, Jiayi Qin, Shanhu Wang, Yang He, Yifeng Du, Bin Yang, Xin Huang, Huiping Han, Yilin Wu, Shuya Liu, Afzal Khan, Zhidong Li, Qianxu Ye, Sheng’an Yang, Ji Ma, Hui Zhang, Xiang Liu, Qingming Chen, Wanbiao Hu, Jing Ma, Jianhong Yi, Jinming Guo*, Shou Peng, Hao Pan*, Liang Wu*, Ce-Wen Nan

Acta Materialia, 294, (2025), 121085

反铁电材料因其独特的双滞回极化特性，在能源存储、机电转换及突触器件等领域展现出重要的应用前景。然而，大量实验研究表明，许多反铁电材料表现出与铁电材料类似的单滞回特性，这一现象的物理机制尚未得到充分阐释。本研究在反铁电唯象模型中，通过引入具有不同反铁电-铁电矫顽场的无序反铁电回线叠加，解释了实验中广泛观察到的“类铁电”电滞回线。在实验方面，我们通过对PbZrO₃和PbHfO₃反铁电薄膜生长条件的精确调控，在材料中引入非均匀缺陷，验证了模型的正确性。

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 PbZrO₃ and PbHfO₃ thin films, by introducing non-uniform local disorder (e.g., defects) via fine-tuning of the film growth condition. 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.

本论文得到了清华大学南策文院士，北京大学彭寿院士、潘豪教授，昆明理工大学易健宏校长，湖北大学郭金明教授，云南大学胡万彪教授等合作者的大力支持，在此一并表示诚挚感谢！