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Abstract Rational design of chiral two‐dimensional hybrid organic–inorganic perovskites is crucial to achieve chiroptoelecronic, spintronic, and ferroelectric applications. Here, an efficient way to manipulate the chiroptoelectronic activity of 2D lead iodide perovskites is reported by forming mixed chiral (R‐ or S‐methylbenzylammonium (R‐MBA⁺or S‐MBA⁺)) and achiral (n‐butylammonium (nBA⁺)) cations in the organic layer. The strongest and flipped circular dichroism signals are observed in (R/S‐MBA_0.5nBA_0.5)₂PbI₄films compared to (R/S‐MBA)₂PbI₄. Moreover, the (R/S‐MBA_0.5nBA_0.5)₂PbI₄films exhibit pseudo‐symmetric, unchanged circularly polarized photoluminescence peak as temperature increases. First‐principles calculations reveal that mixed chiral–achiral cations enhance the asymmetric hydrogen‐bonding interaction between the organic and inorganic layers, causing more structural distortion, thus, larger spin‐polarized band‐splitting than pure chiral cations. Temperature‐dependent powder X‐ray diffraction and pair distribution function structure studies show the compressed intralayer lattice with enlarged interlayer spacing and increased local ordering. Overall, this work demonstrates a new method to tune chiral and chiroptoelectronic properties and reveals their atomic scale structural origins.