Bimodal polymorphic nanodomains in ferroelectric films for giant energy storage
Yuhang Ren, Hongbo Cheng, Jun Ouyang, Onur Kurt, Jianjun Wang, Qinghua Zhang, Yuyao Zhao, Lin Gu, Long‐Qing Chen
Abstract
Enhanced functional responses of ferroelectrics have often been achieved by complex compositional design of a morphotropic or polymorphic phase boundary. Here, we observe a pseudo-linear, ultra-slim polarization-electric field (P-E) hysteresis loop in simple composition, lead-free Ba(Zr,Ti)O3 of up to μm-thick. It features a low remnant polarization and a high maximum polarization after a delayed saturation process with a field-insensitive, thickness-scalable high energy efficiency of ∼90%. This giant energy storage performance is attributed to the self-assembled, bimodal polymorphic nanodomains consisting of two sets of coherent polymorphic nanodomains. The first set of domains has the best-matched, low index {110} interface. They manifest themselves as “entangled nanophases” and dominate in thinner or annealed films. The 2nd set of domains with a high-index {114} interface and an in-plane anisotropy leads to the largest reduction in bulk elastic energy. These domains show as “segregated nanophases” and prevail in as-grown thick films. The presence of multi-polar states in both sets of nanodomains helps reduce the remnant polarization and delay the polarization saturation. Furthermore, the segregated tetragonal phase in-plane nanodomains lead to a larger maximum polarization under a high poling field. Strain engineering of such nanodomain structures provides a promising alternative to chemical compositional design, for the optimization of dielectric thin films used in capacitive energy storage applications.