材料科学
铁电性
氢键
自旋电子学
光致发光
圆二色性
结晶学
凝聚态物理
分子
电介质
光电子学
有机化学
化学
铁磁性
物理
作者
Hao Li,Pranab Sarker,Xiaoyu Zhang,Maxwell W. Terban,Sanjit Ghose,İbrahim Dursun,Mircea Cotlet,Ming‐Xing Li,Yugang Zhang,Yuanze Xu,Shripathi Ramakrishnan,Tao Wei,Deyu Lu,Qiuming Yu
标识
DOI:10.1002/adom.202401782
摘要
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 ( n BA + )) cations in the organic layer. The strongest and flipped circular dichroism signals are observed in (R/S‐MBA 0.5 n BA 0.5 ) 2 PbI 4 films compared to (R/S‐MBA) 2 PbI 4 . Moreover, the (R/S‐MBA 0.5 n BA 0.5 ) 2 PbI 4 films 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.
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