Spatial Structure Design toward Dielectric Elastomers by Separating Charge Centers in Chain Segments

Decorating the backbone of dielectric elastomers (DEs) with polar functionalities is an important practice that increases the total charge quantity of the chain segments, allowing DEs to have high dielectric permittivity (ε′). However, most established methods have struggled with optimizing the electromechanical performance of DEs, as the interactions among their polar functionalities have inevitably deteriorated the network flexibility of DEs. Herein, we present an innovative design concept for homogeneous DEs with superior dielectric properties by incorporating angle-containing monomers as building blocks that enable a flexible "zigzag" chain configuration in the DEs. This configuration, in turn, facilitates the charge separation within the chain segments. Therefore, a substantial increase of ε′ (∼90%) can be achieved while reducing the corresponding Young's modulus, enabling superior and dynamically stable actuation performance in DEs. These findings have the potential to break the longstanding trade-off between dielectric and mechanical performances of conventional DEs upon chemical decorations.