The electric-field-induced phase transition from antipolar to polar structures is at the heart of antiferroelectricity. We demonstrate direct evidence of antiferroelectricity by applying a strong electric field to two antipolar crystals of squaric acid (SQA) and 5,5′-dimethyl-2,2′-bipyridinium chloranilate. The field-induced polarization of SQA is quite large and reasonably explained by the theoretically calculated polarization on the hydrogen-bonded sheet sublattice. The pseudo-tetragonal lattice of SQA permits unique switching topologies that produce two different ferroelectric phases of low and high polarizations. By tilting the applied field direction, the electrical switching mechanism can be attributed to a 90° rotation of the sheet polarization. From the viewpoint of applications, the strong polarization, high switching field, and quite slim hysteresis observed in the polarization versus electric field curve for SQA are advantageous for excellent-efficiency energy storage devices.
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