Enhancing Chiroptoelectronic Activity in Chiral 2D Perovskites via Chiral–Achiral Cation Mixing

Li, Hao; Sarker, Pranab; Zhang, Xiaoyu; Terban, Maxwell W.; Ghose, Sanjit; Dursun, Ibrahim; Cotlet, Mircea; Li, Mingxing; Zhang, Yugang; Xu, Yuanze; Ramakrishnan, Shripathi; Wei, Tao; Lu, Deyu; Yu, Qiuming

doi:10.1002/adom.202401782

Title: Enhancing Chiroptoelectronic Activity in Chiral 2D Perovskites via Chiral–Achiral Cation Mixing

Journal Article · 10 October 2024 · Advanced Optical Materials

DOI: https://doi.org/10.1002/adom.202401782 · OSTI ID:2448245

Li, Hao ^[1];

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^[3]; Ghose, Sanjit ^[4];

^[1];

^[5]; Li, Mingxing ^[5]; Zhang, Yugang ^[5];

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^[1]; Wei, Tao ^[2];

^[5];

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Cornell Univ., Ithaca, NY (United States)
Univ. of South Carolina, Columbia, SC (United States)
Max Planck Institute of Solid State Research, Stuttgart (Germany)
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)

Rational design of chiral two-dimensional hybrid organic–inorganic perovskites is crucial to achieve chiroptoelecronic, spintronic, and ferroelectric applications. Here, in this study, 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)₂PbI₄ films compared to (R/S-MBA)₂PbI₄. Moreover, the (R/S-MBA_0.5nBA_0.5)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.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); National Science Foundation (NSF)

Grant/Contract Number:: SC0012704

OSTI ID:: 2448245

Report Number(s):: BNL--226180-2024-JAAM

Journal Information:: Advanced Optical Materials, Journal Name: Advanced Optical Materials Journal Issue: 35 Vol. 12; ISSN 2195-1071

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Enhancing Chiroptoelectronic Activity in Chiral 2D Perovskites via Chiral–Achiral Cation Mixing

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