Ferroelectric polymer nanocomposites possess exceptional electric properties with respect to the two otherwise uniform phases, which is commonly attributed to the critical role of the matrix–particle interfacial region. However, the structure–property correlation of the interface remains unestablished, and thus, the design of ferroelectric polymer nanocomposite has largely relied on the trial-and-error method. Here, a strategy that combines multi-mode scanning probe microscopy-based electrical characterization and nano-infrared spectroscopy is developed to unveil the local structure–property correlation of the interface in ferroelectric polymer nanocomposites. The results show that the type of surface modifiers decorated on the nanoparticles can significantly influence the local polar-phase content and the piezoelectric effect of the polymer matrix surrounding the nanoparticles. The strongly coupled polar-phase content and piezoelectric effect measured directly in the interfacial region as well as the computed bonding energy suggest that the property enhancement originates from the formation of hydrogen bond between the surface modifiers and the ferroelectric polymer. It is also directly detected that the local domain size of the ferroelectric polymer can impact the energy level and distribution of charge traps in the interfacial region and eventually influence the local dielectric strength.

铁电聚合物纳米复合材料相对于两个均匀相而言具有优异的电性能，这通常归因于基体-颗粒界面区域的关键作用。然而，界面的结构-性能相关性尚未建立，因此，铁电聚合物纳米复合材料的设计在很大程度上依赖于试错法。在这里，开发了一种将基于多模式扫描探针显微镜的电表征和纳米红外光谱相结合的策略，以揭示铁电聚合物纳米复合材料中界面的局部结构-性能相关性。结果表明，纳米颗粒上修饰的表面改性剂类型可以显着影响纳米颗粒周围聚合物基体的局部极性相含量和压电效应。直接在界面区域测量的强耦合极性相含量和压电效应以及计算的键合能表明性能的增强源于表面改性剂和铁电聚合物之间氢键的形成。还直接检测到铁电聚合物的局部域尺寸会影响界面区域中电荷陷阱的能级和分布，并最终影响局部介电强度。