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Pucker up: A metal–organic perovskite with four‐membered‐ring azetidinium cations (see structure) exhibited a very broad and unprecedentedly large dielectric peak near 280 K. It is highly possible that the ring‐puckering instability of the four‐membered‐ring ammonium cation plays an essential role in inducing the change of the lattice symmetry and the extraordinarily large dielectric anomaly.
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