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Using first-principles calculations, the phase diagrams of polyvinylidene fluoride (PVDF) and its copolymers under an applied electric field are studied and phase transitions between their nonpolar α and polar β phases are discussed. The results show that the degree of copolymerization is a crucial parameter controlling the structural phase transition. In particular, for tetrafluoroethylene (TeFE) concentration above 12%, PVDF–TeFE is stabilized in the β phase, whereas the α phase is stable for lower concentrations. As larger electric fields are applied, domains with smaller concentrations (\leq 12%) undergo a transition from the α to the β phase until a breakdown field of ~600 MV m−1 is reached. These structural phase transitions can be exploited for efficient storage of electrical energy.

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