Abstract
Ferroelectrics hold significant promise for a wide range of applications owing to their spontaneous polarization characteristics. Despite exhibiting multiple polarization mechanisms that demonstrate significant potential for electromagnetic functional materials, the practical deployment of ferroelectric polymers has been inhibited by the lack of precise control over polymer chains at the atomic scale and the relatively low stability of the polar phase. Here, a procedure of fortifying the ferroelectric polyvinylidene fluoride phase is proposed by the facet modulation, achieving stable ferroelectric polymer through engineering the interaction between the inorganic rigid crystal facets and organic flexible molecular chains at the atomic scale. The constructed polar ferroelectric polymers composite systems exhibit a broad distribution of relaxation times along with multi-polarization characteristics from megahertz to terahertz frequencies. The composite system mitigates the apparent loss-bandwidth trade-off, thereby achieving broadband polarization properties across multiple frequency bands while maintaining a dissipation efficiency above 99.9%. The demonstrated approach presents a breakthrough in achieving the stable ferroelectric polymers through facet-induced stabilization, providing deep insights for the development of high-performance electromagnetic functional materials.