Hao Li, Pranab Sarker, Xiaoyu Zhang, Maxwell W. Terban, Sanjit Ghose, Ibrahim Dursun, Mircea Cotlet, Mingxing Li, Yugang Zhang, Yuanze Xu, Shripathi Ramakrishnan, Tao Wei, Deyu Lu, Qiuming Yu
{"title":"Enhancing Chiroptoelectronic Activity in Chiral 2D Perovskites via Chiral–Achiral Cation Mixing","authors":"Hao Li, Pranab Sarker, Xiaoyu Zhang, Maxwell W. Terban, Sanjit Ghose, Ibrahim Dursun, Mircea Cotlet, Mingxing Li, Yugang Zhang, Yuanze Xu, Shripathi Ramakrishnan, Tao Wei, Deyu Lu, Qiuming Yu","doi":"10.1002/adom.202401782","DOIUrl":null,"url":null,"abstract":"<p>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<sup>+</sup> or S-MBA<sup>+</sup>)) and achiral (<i>n</i>-butylammonium (<i>n</i>BA<sup>+</sup>)) cations in the organic layer. The strongest and flipped circular dichroism signals are observed in (R/S-MBA<sub>0.5</sub><i>n</i>BA<sub>0.5</sub>)<sub>2</sub>PbI<sub>4</sub> films compared to (R/S-MBA)<sub>2</sub>PbI<sub>4</sub>. Moreover, the (R/S-MBA<sub>0.5</sub><i>n</i>BA<sub>0.5</sub>)<sub>2</sub>PbI<sub>4</sub> 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.</p>","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":"12 35","pages":""},"PeriodicalIF":8.0000,"publicationDate":"2024-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Advanced Optical Materials","FirstCategoryId":"88","ListUrlMain":"https://onlinelibrary.wiley.com/doi/10.1002/adom.202401782","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
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-MBA0.5nBA0.5)2PbI4 films compared to (R/S-MBA)2PbI4. Moreover, the (R/S-MBA0.5nBA0.5)2PbI4 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.
期刊介绍:
Advanced Optical Materials, part of the esteemed Advanced portfolio, is a unique materials science journal concentrating on all facets of light-matter interactions. For over a decade, it has been the preferred optical materials journal for significant discoveries in photonics, plasmonics, metamaterials, and more. The Advanced portfolio from Wiley is a collection of globally respected, high-impact journals that disseminate the best science from established and emerging researchers, aiding them in fulfilling their mission and amplifying the reach of their scientific discoveries.