Large-Area Flexible Memory Arrays of Oriented Molecular Ferroelectric Single Crystals with Nearly Saturated Polarization.

Molecular ferroelectrics (MFs) have been proven to demonstrate excellent properties even comparable to those of inorganic counterparts usually with heavy metals. However, the validation of their device applications is still at the infant stage. The polycrystalline feature of conventionally obtained MF films, the patterning challenges for microelectronics and the brittleness of crystalline films significantly hinder their development for organic integrated circuits, as well as emerging flexible electronics. Here, a large-area flexible memory array is demonstrated of oriented molecular ferroelectric single crystals (MFSCs) with nearly saturated polarization. Highly-uniform MFSC arrays are  prepared on large-scale substrates including Si wafers and flexible substrates using an asymmetric-wetting and microgroove-assisted coating (AWMAC) strategy. Resultant flexible memory arrays exhibit excellent nonvolatile memory properties with a low-operating voltage of <5 V, i.e., nearly saturated ferroelectric polarization (6.5 µC cm-2 ), and long bending endurance (>103 ) under various bending radii. These results may open an avenue for scalable flexible MF electronics with high performance.

[1]  Ruipeng Li,et al.  Relaxor ferroelectric polymer exhibits ultrahigh electromechanical coupling at low electric field , 2022, Science.

[2]  Z. Qiu,et al.  Single-Crystalline Thin-Film Memory Arrays of Molecular Ferroelectrics with Ultralow Operation Voltages , 2022, ACS Materials Letters.

[3]  Hasnain Mehdi Jafri,et al.  Improper molecular ferroelectrics with simultaneous ultrahigh pyroelectricity and figures of merit , 2021, Science Advances.

[4]  Pooi See Lee,et al.  Ferroelastic-switching-driven large shear strain and piezoelectricity in a hybrid ferroelectric , 2020, Nature Materials.

[5]  H. Hwang,et al.  Effect of dead layers on the ferroelectric property of ultrathin HfZrOx film , 2020, Applied Physics Letters.

[6]  Min Koo,et al.  Soft Ferroelectrics Enabling High‐Performance Intelligent Photo Electronics , 2020, Advanced materials.

[7]  Z. Qiu,et al.  Wafer‐Scale Diisopropylammonium Bromide Films for Low‐Power Lateral Organic Ferroelectric Capacitors , 2020, Advanced Electronic Materials.

[8]  R. Xiong,et al.  Methylphosphonium Tin Bromide: A 3D Perovskite Molecular Ferroelectric Semiconductor , 2020, Advanced materials.

[9]  Jiansheng Jie,et al.  High-resolution patterning of organic semiconductor single crystal arrays for high-integration organic field-effect transistors , 2020 .

[10]  Yuan‐Yuan Tang,et al.  Six-Fold Vertices in a Single-Component Organic Ferroelectric with Most Equivalent Polarization Directions. , 2020, Journal of the American Chemical Society.

[11]  Xitao Liu,et al.  Ferroelectricity-Driven Self-Powered Ultraviolet Photodetection with Strong Polarization-Sensitivity in a Two-Dimensional Halide Hybrid Perovskite. , 2020, Angewandte Chemie.

[12]  Xiao-Gang Chen,et al.  The Soft Molecular Polycrystalline Ferroelectric Realized by Fluorination Effect. , 2020, Journal of the American Chemical Society.

[13]  Jiansheng Jie,et al.  A Microchannel‐Confined Crystallization Strategy Enables Blade Coating of Perovskite Single Crystal Arrays for Device Integration , 2020, Advanced materials.

[14]  Yingjie Zhao,et al.  Layered‐Perovskite Nanowires with Long‐Range Orientational Order for Ultrasensitive Photodetectors , 2020, Advanced materials.

[15]  R. Xiong,et al.  The First 2D Homochiral Lead Iodide Perovskite Ferroelectrics: [R‐ and S‐1‐(4‐Chlorophenyl)ethylammonium]2PbI4 , 2019, Advanced materials.

[16]  R. Xiong,et al.  Directional Intermolecular Interactions for Precise Molecular Design of a High- Tc Multiaxial Molecular Ferroelectric. , 2019, Journal of the American Chemical Society.

[17]  Peng-Fei Li,et al.  Metal-free three-dimensional perovskite ferroelectrics , 2018, Science.

[18]  X. Zhang,et al.  Single-crystalline layered metal-halide perovskite nanowires for ultrasensitive photodetectors , 2018, Nature Electronics.

[19]  S. Lanceros‐Méndez,et al.  Electroactive poly(vinylidene fluoride)-based structures for advanced applications , 2018, Nature Protocols.

[20]  Z. Qiu,et al.  Space‐Charge‐Stabilized Ferroelectric Polarization in Self‐Oriented Croconic Acid Films , 2018 .

[21]  B. Zhang,et al.  Regular Aligned 1D Single-Crystalline Supramolecular Arrays for Photodetectors. , 2018, Small.

[22]  Peng-Fei Li,et al.  Large Piezoelectric Effect in a Lead-Free Molecular Ferroelectric Thin Film. , 2017, Journal of the American Chemical Society.

[23]  Yu-Meng You,et al.  A Molecular Polycrystalline Ferroelectric with Record‐High Phase Transition Temperature , 2017, Advanced materials.

[24]  Jinlan Wang,et al.  An organic-inorganic perovskite ferroelectric with large piezoelectric response , 2017, Science.

[25]  Xu Han,et al.  PVDF‐Based Ferroelectric Polymers in Modern Flexible Electronics , 2017 .

[26]  Takayoshi Nakamura,et al.  Quinuclidinium salt ferroelectric thin-film with duodecuple-rotational polarization-directions , 2017, Nature Communications.

[27]  Yu-Meng You,et al.  Ultrafast Polarization Switching in a Biaxial Molecular Ferroelectric Thin Film: [Hdabco]ClO4. , 2016, Journal of the American Chemical Society.

[28]  Yu-Meng You,et al.  Molecular Ferroelectric with Most Equivalent Polarization Directions Induced by the Plastic Phase Transition. , 2016, Journal of the American Chemical Society.

[29]  T. Inabe,et al.  Directionally tunable and mechanically deformable ferroelectric crystals from rotating polar globular ionic molecules. , 2016, Nature chemistry.

[30]  Jiansheng Jie,et al.  An Inherent Multifunctional Sellotape Substrate for High‐Performance Flexible and Wearable Organic Single‐Crystal Nanowire Array‐Based Transistors , 2016 .

[31]  V. Garcia,et al.  Tunnel electroresistance through organic ferroelectrics , 2016, Nature Communications.

[32]  Mengyuan Li,et al.  The negative piezoelectric effect of the ferroelectric polymer poly(vinylidene fluoride). , 2016, Nature materials.

[33]  Toshikazu Yamada,et al.  Few‐Volt Operation of Printed Organic Ferroelectric Capacitor , 2015, Advanced materials.

[34]  H. Xin,et al.  Interfacing Solution‐Grown C60 and (3‐Pyrrolinium)(CdCl3) Single Crystals for High‐Mobility Transistor‐Based Memory Devices , 2015, Advanced materials.

[35]  P. Blom,et al.  Polarization fatigue of organic ferroelectric capacitors , 2014, Scientific Reports.

[36]  Jiangyu Li,et al.  A molecular ferroelectric thin film of imidazolium perchlorate that shows superior electromechanical coupling. , 2014, Angewandte Chemie.

[37]  K. Awaga,et al.  Storage of an electric field for photocurrent generation in ferroelectric-functionalized organic devices , 2014, Nature Communications.

[38]  J. Hone,et al.  Elastically strained nanowires and atomic sheets , 2014 .

[39]  D. Bonnell Ferroelectric Organic Materials Catch Up with Oxides , 2013, Science.

[40]  G. Giovannetti,et al.  Diisopropylammonium Bromide Is a High-Temperature Molecular Ferroelectric Crystal , 2013, Science.

[41]  P. Jeon,et al.  MoS2 nanosheets for top-gate nonvolatile memory transistor channel. , 2012, Small.

[42]  Kang L. Wang,et al.  Room-temperature ferroelectricity in supramolecular networks of charge-transfer complexes , 2012, Nature.

[43]  R. Xiong,et al.  Diisopropylammonium Chloride: A Ferroelectric Organic Salt with a High Phase Transition Temperature and Practical Utilization Level of Spontaneous Polarization , 2011, Advanced materials.

[44]  Klaus Reimann,et al.  Multilevel Information Storage in Ferroelectric Polymer Memories , 2011, Advanced materials.

[45]  Y. Tokura,et al.  Above-room-temperature ferroelectricity in a single-component molecular crystal. , 2010, Nature.

[46]  Nicola A. Spaldin,et al.  Origin of the dielectric dead layer in nanoscale capacitors , 2006, Nature.