Synergistic design of a new PbHfO 3 -based antiferroelectric solid solution with high energy storage and large strain performances under low electric fields

Antiferroelectric (AFE) materials have gained significant attention due to their potential multifunctionality. However, prototypical AFE materials, such as PbHfO 3 , suffer from poor sinterability, complex structures, and a high critical electric field, making it difficult for them to achieve expected performances. Here we adopt a synergistic design strategy, namely by inducing ferroelectrically active ions into the PbHfO 3 structural matrix to soften the AFE order and induce a large maximum polarization, to enable the development of novel PbHfO 3 -based AFE materials of high performance suitable for applications under low electric fields. To implement this strategy, a novel solid solution of (1 − x )PbHfO 3 – x Pb(Zn 1/2 W 1/2 )O 3 is designed and prepared by the solid-state reaction method. Its crystal structure, microstructures, energy storage and strain performances, and phase transition behaviors are systematically investigated from both experimental and theoretical aspects. The resulting material exhibits a high recoverable energy storage density of 5.03 J cm −3 and a large strain of 0.60% under a relatively low electric field of 200 kV cm −1 , which proves the effectiveness of our synergistic strategy. Phenomenological modeling investigation associates these performances with the sharp jump in induced polarization and strain, which is consistent with the experimental results. This work not only results in a novel AFE candidate material for high energy storage and strain applications but also, more importantly, opens up a new way to design high-performance AFE materials with multifunctionality via softening the AFE order.