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The lead‐free hybrid perovskite piezoelectrics possess advantages of easy processing, light weight, and low‐toxicity over inorganic ceramics. However, the lack of understanding in structure–property relationships hinders exploration of new molecular piezoelectric crystals with excellent performances. Herein, by introducing chiral α‐phenylethylammonium (α‐PEA+) cations into bismuth‐based hybrid halides,...
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