Dielectric elastomer actuators are stretchable capacitors capable of a musclelike actuation when charged. They will one day be used to replace malfunctioning muscles supposing the driving voltage can be reduced below 24 V. This focus here is on polar dielectric elastomers and their behavior under an electric field. Emphasis is placed on all the features that are correlated with the molecular structure, its synthetic realization, and its impact on properties. Regarding the polymer class, the focus, to some degree, is on polysiloxanes because of their attractively low glass transition temperatures. This enables introduction of highly polar groups to the backbone while maintaining soft elastic properties. The goal is to provide a few guidelines for future research in this emerging field that may be useful for those considering entering this fascinating endeavor. Because of the large number of materials available, a few restrictions in the selection have to be applied.
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