Lone pair expression in fluorinated two-dimensional hybrid perovskite enables multiaxial ferroelectricity and nonlinear optical response

Hao-Fei Ni, Qi-Fang Zhou, Jia-Qi Luo, Gele Teri, Lei Pan, Lou-Kai Ye, Qiang-Qiang Jia, Pei-Zhi Huang, Pei-Guo Liu, Chang-Feng Wang, Zhi-Xu Zhang (), Da-Wei Fu () and Yi Zhang ()
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Hao-Fei Ni: Zhejiang Normal University
Qi-Fang Zhou: Zhejiang Normal University
Jia-Qi Luo: Zhejiang Normal University
Gele Teri: Zhejiang Normal University
Lei Pan: Zhejiang Normal University
Lou-Kai Ye: Zhejiang Normal University
Qiang-Qiang Jia: Zhejiang Normal University
Pei-Zhi Huang: Zhejiang Normal University
Pei-Guo Liu: Zhejiang Normal University
Chang-Feng Wang: Zhejiang Normal University
Zhi-Xu Zhang: Zhejiang Normal University
Da-Wei Fu: Zhejiang Normal University
Yi Zhang: Zhejiang Normal University

Nature Communications, 2025, vol. 16, issue 1, 1-10

Abstract: Abstract Two-dimensional (2D) hybrid organic-inorganic perovskites (HOIPs) with tunable octahedra are promising for flexible devices due to spontaneous-polarization-driven functionalities like ferroelectric memory, piezoelectric sensing and optical switches. However, achieving large spontaneous polarization and strong second harmonic generation (SHG) remains challenging for 2D HOIP ferroelectrics. Here, we report a 2D HOIP ferroelectric (4,4-difluoropiperidinium)2GeBr4 designed by molecular fluorination. Remarkably, (4,4-difluoropiperidinium)2GeBr4 exhibits large saturation polarization (>15 μC/cm2), high Curie temperature (401 K) and the strongest SHG intensity among 2D HOIP ferroelectrics (about 6.2 times of KH2PO4). These properties arise from the synergy of two mechanisms: the 4s2 lone pair on Ge2+ and the orientational ordering of 4,4-difluoropiperidinium cations. Moreover, (4,4-difluoropiperidinium)2GeBr4 features eight equivalent polarization directions (the maximum number among reported 2D HOIP ferroelectrics), enabling its composite (4,4-difluoropiperidinium)2GeBr4@thermoplastic polyurethane device to exhibit prominent piezoelectric sensing. Our work offers a reliable route to high-performance 2D hybrid ferroelectrics and highlights their potential in flexible devices.

Date: 2025
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DOI: 10.1038/s41467-025-63134-6

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