Flexoelectricity in soft elastomers and the molecular mechanisms underpinning the design and emergence of giant flexoelectricity.

Soft robotics requires materials that are capable of large deformation and amenable to actuation with external stimuli such as electric fields. Energy harvesting, biomedical devices, flexible electronics, and sensors are some other applications enabled by electroactive soft materials. The phenomenon of flexoelectricity is an enticing alternative that refers to the development of electric polarization in dielectrics when subjected to strain gradients. In particular, flexoelectricity offers a direct linear coupling between a highly desirable deformation mode (flexure) and electric stimulus. Unfortunately, barring some exceptions, the flexoelectric effect is quite weak and rather substantial bending curvatures are required for an appreciable electromechanical response. Most experiments in the literature appear to confirm modest flexoelectricity in polymers although perplexingly, a singular work has measured a "giant" effect in elastomers under some specific conditions. Due to the lack of an understanding of the microscopic underpinnings of flexoelectricity in elastomers and a commensurate theory, it is not currently possible to either explain the contradictory experimental results on elastomers or pursue avenues for possible design of large flexoelectricity. In this work, we present a statistical-mechanics theory for the emergent flexoelectricity of elastomers consisting of polar monomers. The theory is shown to be valid in broad generality and leads to key insights regarding both giant flexoelectricity and material design. In particular, the theory shows that, in standard elastomer networks, combining stretching and bending is a mechanism for obtaining giant flexoelectricity, which also explains the aforementioned, surprising experimental discovery.