Unprecedented 2D Homochiral Hybrid Lead‐Iodide Perovskite Thermochromic Ferroelectrics with Ferroelastic Switching

Chiral perovskites have emerged as a significant class of materials showing promising optoelectronic and spintronic applications. Reports of chiral perovskite ferroelectrics, however, have been scarce. In this work, we have successfully synthesized homochiral lead-iodide perovskite ferroelectrics [(R)-N-(1-phenylethyl)ethane-1,2-diaminium]PbI₄ and [(S)-N-(1-phenylethyl)ethane-1,2-diaminium]PbI₄ by introducing a methyl group into the organic cation of the parent (N-benzylethane-1,2-diaminium)PbI₄ . Vibrational circular dichroism spectra identify the chiral mirroring relationship. They both undergo 222F2-type paraelectric-ferroelectric behavior at around 378 K coupled with clear ferroelastic domain "ON/OFF" switching. Besides, they exhibit an evident thermochromism with color change from orange-yellow to orange-red. To our knowledge, the discovery of integrated ferroelectricity, ferroelasticity, and reversible thermochromism in chiral perovskites is unprecedented.