Controllable Shifts in Threshold Voltage of Top‐Gate Polymer Field‐Effect Transistors for Applications in Organic Nano Floating Gate Memory

Organic field‐effect transistor (FET) memory is an emerging technology with the potential to realize light‐weight, low‐cost, flexible charge storage media. Here, solution‐processed poly[9,9‐dioctylfluorenyl‐2,7‐diyl]‐co‐(bithiophene)] (F8T2) nano floating gate memory (NFGM) with a top‐gate/bottom‐contact device configuration is reported. A reversible shift in the threshold voltage (V_Th) and reliable memory characteristics was achieved by the incorporation of thin Au nanoparticles (NPs) as charge storage sites for negative charges (electrons) at the interface between polystyrene and cross‐linked poly(4‐vinylphenol). The F8T2 NFGM showed relatively high field‐effect mobility (µ_FET) (0.02 cm² V^?1 s^?1) for an amorphous semiconducting polymer with a large memory window (ca. 30 V), a high on/off ratio (more than 10⁴) during writing and erasing with an operation voltage of 80 V of gate bias in a relatively short timescale (less than 1 s), and a retention time of a few hours. This top‐gated polymer NFGM could be used as an organic transistor memory element for organic flash memory.     

Electron‐Rich Alcohol‐Soluble Neutral Conjugated Polymers as Highly Efficient Electron‐Injecting Materials for Polymer Light‐Emitting Diodes

We report the design and synthesis of three alcohol‐soluble neutral conjugated polymers, poly[9,9‐bis(2‐(2‐(2‐diethanolaminoethoxy) ethoxy)ethyl)fluorene] (PF‐OH), poly[9,9‐bis(2‐(2‐(2‐diethanol‐aminoethoxy)ethoxy)ethyl)fluorene‐alt‐4,4′‐phenylether] (PFPE‐OH) and poly[9,9‐bis(2‐(2‐(2‐diethanolaminoethoxy) ethoxy)ethyl)fluorene‐alt‐benzothiadizole] (PFBT‐OH) with different conjugation length and electron affinity as highly efficient electron injecting and transporting materials for polymer light‐emitting diodes (PLEDs). The unique solubility of these polymers in polar solvents renders them as good candidates for multilayer solution processed PLEDs. Both the fluorescent and phosphorescent PLEDs based on these polymers as electron injecting/transporting layer (ETL) were fabricated. It is interesting to find that electron‐deficient polymer (PFBT‐OH) shows very poor electron‐injecting ability compared to polymers with electron‐rich main chain (PF‐OH and PFPE‐OH). This phenomenon is quite different from that obtained from conventional electron‐injecting materials. Moreover, when these polymers were used in the phosphorescent PLEDs, the performance of the devices is highly dependent on the processing conditions of these polymers. The devices with ETL processed from water/methanol mixed solvent showed much better device performance than the devices processed with methanol as solvent. It was found that the erosion of the phosphorescent emission layer could be greatly suppressed by using water/methanol mixed solvent for processing the polymer ETL. The electronic properties of the ETL could also be influenced by the processing conditions. This offers a new avenue to improve the performance of phosphorescent PLEDs through manipulating the processing conditions of these conjugated polymer ETLs.     

Printed,Flexible, Organic Nano‐Floating‐Gate Memory: Effects of Metal Nanoparticles and Blocking Dielectrics on Memory Characteristics

The effects of using a blocking dielectric layer and metal nanoparticles (NPs) as charge‐trapping sites on the characteristics of organic nano‐floating‐gate memory (NFGM) devices are investigated. High‐performance NFGM devices are fabricated using the n‐type polymer semiconductor, poly{[N,N′‐bis(2‐octyldodecyl)‐naphthalene‐1,4,5,8‐bis(dicarboximide)‐2,6‐diyl]‐alt‐5,5′‐(2,2′‐bithiophene)} (P(NDI2OD‐T2)), and various metal NPs. These NPs are embedded within bilayers of various polymer dielectrics (polystyrene (PS)/poly(4‐vinyl phenol) (PVP) and PS/poly(methyl methacrylate) (PMMA)). The P(NDI2OD‐T2) organic field‐effect transistor (OFET)‐based NFGM devices exhibit high electron mobilities (0.4–0.5 cm² V^?1 s^?1) and reliable non‐volatile memory characteristics, which include a wide memory window (≈52 V), a high on/off‐current ratio (I_on/I_off ≈ 10⁵), and a long extrapolated retention time (>10⁷ s), depending on the choice of the blocking dielectric (PVP or PMMA) and the metal (Au, Ag, Cu, or Al) NPs. The best memory characteristics are achieved in the ones fabricated using PMMA and Au or Ag NPs. The NFGM devices with PMMA and spatially well‐distributed Cu NPs show quasi‐permanent retention characteristics. An inkjet‐printed flexible P(NDI2OD‐T2) 256‐bit transistor memory array (16 × 16 transistors) with Au‐NPs on a polyethylene naphthalate substrate is also fabricated. These memory devices in array exhibit a high I_on/I_off (≈10^{4 ± 0.85}), wide memory window (≈43.5 V ± 8.3 V), and a high degree of reliability.     

High‐Performance Top‐Gated Organic Field‐Effect Transistor Memory using Electrets for Monolithic Printed Flexible NAND Flash Memory

High‐performance top‐gated organic field‐effect transistor (OFET) memory devices using electrets and their applications to flexible printed organic NAND flash are reported. The OFETs based on an inkjet‐printed p‐type polymer semiconductor with efficiently chargeable dielectric poly(2‐vinylnaphthalene) (PVN) and high‐k blocking gate dielectric poly(vinylidenefluoride‐trifluoroethylene) (P(VDF‐TrFE)) shows excellent non‐volatile memory characteristics. The superior memory characteristics originate mainly from reversible charge trapping and detrapping in the PVN electret layer efficiently in low‐k/high‐k bilayered dielectrics. A strategy is devised for the successful development of monolithically inkjet‐printed flexible organic NAND flash memory through the proper selection of the polymer electrets (PVN or PS), where PVN/‐ and PS/P(VDF‐TrFE) devices are used as non‐volatile memory cells and ground‐ and bit‐line select transistors, respectively. Electrical simulations reveal that the flexible printed organic NAND flash can be possible to program, read, and erase all memory cells in the memory array repeatedly without affecting the non‐selected memory cells.     

Organic nonvolatile memory devices utilizing intrinsic charge-trapping phenomena in an n-type polymer semiconductor

Charge trapping is an undesirable phenomenon and a common challenge in the operation of n-channel organic field-effect transistors. Herein, we exploit charge trapping in an n-type semiconducting poly (naphthalene diimide-alt-biselenophene) (PNDIBS) as the key operational mechanism to develop high performance, nonvolatile, electronic memory devices. The PNDIBS-based field-effect transistor memory devices were programmed at 60 V and they showed excellent charge-trapping and de-trapping characteristics, which could be cycled more than 200 times with a current ratio of 10³ between the two binary states. Programmed data could be retained for 10³ s with a memory window of 28 V. This is a record performance for n-channel organic transistor with inherent charge-trapping capability without using external charge trapping agents. However, the memory device performance was greatly reduced, as expected, when the n-type polymer semiconductor was end-capped with phenyl groups to reduce the trap density. These results show that the trap density of n-type semiconducting polymers could be engineered to control the inherent charge-trapping capability and device performance for developing high-performance low-cost memory devices.     

High‐Mobility Air‐Stable Naphthalene Diimide‐Based Copolymer Containing Extended π‐Conjugation for n‐Channel Organic Field Effect Transistors

A high‐performance naphthalene diimide (NDI)‐based conjugated polymer for use as the active layer of n‐channel organic field‐effect transistors (OFETs) is reported. The solution‐processable n‐channel polymer is systematically designed and synthesized with an alternating structure of long alkyl substituted‐NDI and thienylene–vinylene–thienylene units (PNDI‐TVT). The material has a well‐controlled molecular structure with an extended π‐conjugated backbone, with no increase in the LUMO level, achieving a high mobility and highly ambient stable n‐type OFET. The top‐gate, bottom‐contact device shows remarkably high electron charge‐carrier mobility of up to 1.8 cm² V^?1 s^?1 (I_on/I_off = 10⁶) with the commonly used polymer dielectric, poly(methyl methacrylate) (PMMA). Moreover, PNDI‐TVT OFETs exhibit excellent air and operation stability. Such high device performance is attributed to improved π–π intermolecular interactions owing to the extended π‐conjugation, apart from the improved crystallinity and highly interdigitated lamellar structure caused by the extended π–π backbone and long alkyl groups.     

Nonvolatile Ferroelectric P(VDF‐TrFE) Memory Transistors Based on Inkjet‐Printed Organic Semiconductor

Nonvolatile ferroelectric poly(vinylidene fluoride‐co‐trifluoroethylene) memory based on an organic thin‐film transistor with inkjet‐printed dodecyl‐substituted thienylenevinylene‐thiophene copolymer (PC12TV12T) as the active layer is developed. The memory window is 4.5 V with a gate voltage sweep of ?12.5 V to 12.5 V. The field effect mobility, on/off ratio, and gate leakage current are 0.1 cm²/Vs, 10⁵, and 10^?10 A, respectively. Although the retention behaviors should be improved and optimized, the obtained characteristics are very promising for future flexible electronics.     

High‐Performance Organic Transistor Memory Elements with Steep Flanks of Hysteresis

High‐performance organic transistor memory elements with donor‐polymer blends as buffer layers are presented. These organic memory transistors have steep flanks of hysteresis with an ON/OFF memory ratio of up to 2 × 10⁴, and a retention time in excess of 24 h. Inexpensive materials such as poly(methyl methacrylate), ferrocene and copper phthalocyanine are used for the device fabrication, providing a convenient approach of producing organic memory transistors at low cost and high efficiency.     

High Performance Multi‐Level Non‐Volatile Polymer Memory with Solution‐Blended Ferroelectric Polymer/High‐k Insulators for Low Voltage Operation

Polymer ferroelectric‐gate field effect transistors (Fe‐FETs) employing ferroelectric polymer thin films as gate insulators are highly attractive as a next‐generation non‐volatile memory. Furthermore, polymer Fe‐FETs have been recently of interest owing to their capability of storing data in more than 2 states in a single device, that is, they have multi‐level cell (MLC) operation potential for high density data storage. However, among a variety of technological issues of MLC polymer Fe‐FETs, the requirement of high voltage for cell operation is one of the most urgent problems. Here, a low voltage operating MLC polymer Fe‐FET memory with a high dielectric constant (k) ferroelectric polymer insulator is presented. Effective enhancement of capacitance of the ferroelectric gate insulator layer is achieved by a simple binary solution‐blend of a ferroelectric poly(vinylidene fluoride‐co‐trifluoroethylene) (PVDF‐TrFE) (k ≈ 8) with a relaxer high‐k poly(vinylidene‐fluoride–trifluoroethylene–chlorotrifluoroethylene) (PVDF‐TrFE‐CTFE) (k ≈ 18). At optimized conditions, a ferroelectric insulator with a PVDF‐TrFE/PVDF‐TrFE‐CTFE (10/5) blend composition enables the discrete six‐level multi‐state operation of a MLC Fe‐FET at a gate voltage sweep of ±18 V with excellent data retention and endurance of each state of more than 10⁴ s and 120 cycles, respectively.     

Electrical bistability,negative differential resistance and carrier transport in flexible organic memory device based on polymer bilayer structure

Bistable nonvolatile memory devices containing two different layers of polymers, viz. MEH-PPV (poly[2-methoxy-5-(2′-ethyl-hexyloxy)-1,4-phenyl vinylene]) and PEDOT:PSS (poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate)) has been fabricated by a simple spin-coating technique on flexible polyimide (PI) substrates with a structure Al/MEH-PPV/PEDOT:PSS/Ag-Pd/PI. The current–voltage measurements of the as-fabricated devices showed a nonvolatile electrical bistability with electric field induced charge transfer through the polymer layers and negative differential resistance (NDR) which is attributed to the charge trapping in the MEH-PPV layer. The current ON/OFF ratio between the high-conducting state (ON state) and low-conducting state (OFF state) is found to be of the order of 10³ at room temperature which is comparable to organic field effect transistor based memory devices. We propose that such an improvement of rectification ratio (ON/OFF ratio) is caused due to the inclusion of PEDOT:PSS, which serves as a conducting current path for carrier transport; however, NDR is an effect of the trapped charges in the MEH-PPV electron confinement layer. The device shows excellent stability over 10⁴ s without any significant degradation under continuous readout testing in both the ON and OFF states. The carrier transport mechanism of the fabricated organic bistable device has been explained on the basis of different conduction mechanisms such as thermionic emission, space-charge-limited conduction, and Fowler–Nordheim tunneling. A band diagram is proposed to explain the charge transport phenomena. These bilayer structures are free from the drawbacks of the single organic layer based memory devices where the phase separation between the nanoparticles and polymers leads to the degradation of device stability and lifetime.     

Ultrathin,Organic, Semiconductor/Polymer Blends by Scanning Corona‐Discharge Coating for High‐Performance Organic Thin‐Film Transistors

A new thin‐film coating process, scanning corona‐discharge coating (SCDC), to fabricate ultrathin tri‐isopropylsilylethynyl pentacene (TIPS‐PEN)/amorphous‐polymer blend layers suitable for high‐performance, bottom‐gate, organic thin‐film transistors (OTFTs) is described. The method is based on utilizing the electrodynamic flow of gas molecules that are corona‐discharged at a sharp metallic tip under a high voltage and subsequently directed towards a bottom electrode. With the static movement of the bottom electrode, on which a blend solution of TIPS‐PEN and an amorphous polymer is deposited, SCDC provides an efficient route to produce uniform blend films with thicknesses of less than one hundred nanometers, in which the TIPS‐PEN and the amorphous polymer are vertically phase‐separated into a bilayered structure with a single‐crystalline nature of the TIPS‐PEN. A bottom‐gate field‐effect transistor with a blend layer of TIPS‐PEN/polystyrene (PS) (90/10 wt%) operated at ambient conditions, for example, indeed exhibits a highly reliable device performance with a field‐effect mobility of approximately 0.23 cm² V^?1 s^?1: two orders of magnitude greater than that of a spin‐coated blend film. SCDC also turns out to be applicable to other amorphous polymers, such as poly(α‐methyl styrene) and poly(methyl methacrylate) and, readily combined with the conventional transfer‐printing technique, gives rise to micropatterned arrays of TIPS‐PEN/polymer films.     

Controlled growth of a graphene charge-floating gate for organic non-volatile memory transistors

We report memory application for graphene as a floating gate in organic thin-film transistor (OTFT) structure. For graphene floating gate, we demonstrate a simpler synthesis method to form a discrete graphene layer by controlling the growth time during a conventional CVD process. The resulting organic memory transistor with the discrete graphene charge-storage layer is evaluated. The device was demonstrated based on solution-processed tunneling dielectric layers and evaporated pentacene organic semiconductor. The resulting devices exhibited programmable memory characteristics, including threshold voltage shifts (∼28 V) in the programmed/erased states when an appropriate gate voltage was applied. They also showed an estimated long data retention ability and program/erase cycles endurance more than 100 times with reliable non-volatile memory properties although operated without encapsulation and in an ambient condition.     

Coordinatable and High Charge‐Carrier‐Mobility Water‐Soluble Conjugated Copolymers for Effective Aqueous‐Processed Polymer–Nanocrystal Hybrid Solar Cells and OFET Applications

A water‐soluble conjugated polymer (WCP) poly[(3,4‐dibromo‐2,5‐thienylene vinylene)‐co‐(p‐phenylene‐vinylene)] (PBTPV), containing thiophene rings with high charge‐carrier mobility and benzene rings with excellent solubility is designed and prepared through Wessling polymerization. The PBTPV precursor can be easily processed by employing water or alcohols as the solvents, which are clean, environmentally friendly, and non‐toxic compared with the highly toxic organic solvents such as chloroform and chlorobenzene. As a novel photoelectric material, PBTPV presents excellent hole‐transport properties with a carrier mobility of 5 × 10^?4 cm² V^?1 s^?1 measured in an organic field‐effect transistor device. By integrating PBTPV with aqueous CdTe nanocrystals (NCs) to produce the active layer of water‐processed hybrid solar cells, the devices exhibit effective power conversion efficiency up to 3.3%. Moreover, the PBTPV can form strong coordination interactions with the CdTe NCs through the S atoms on the thiophene rings, and effective coordination with other nanoparticles can be reasonably expected.     

Anisotropy of Charge Transport in a Uniaxially Aligned and Chain‐Extended,High‐Mobility,Conjugated Polymer Semiconductor

Charge transport in the ribbon phase of poly(2,5‐bis(3‐alkylthiophen‐2‐yl)thieno[3,2‐b]thiophene) (PBTTT)—one of the most highly ordered, chain‐extended crystalline microstructures available in a conjugated polymer semiconductor—is studied. Ribbon‐phase PBTTT has previously been found not to exhibit high carrier mobilities, but it is shown here that field‐effect mobilities depend strongly on the device architecture and active interface. When devices are constructed such that the ribbon‐phase films are in contact with either a polymer gate dielectric or an SiO₂ gate dielectric modified by a hydrophobic, self‐assembled monolayer, high mobilities of up to 0.4 cm² V^?1 s^?1 can be achieved, which is comparable to those observed previously in terrace‐phase PBTTT. In uniaxially aligned, zone‐cast films of ribbon‐phase PBTTT the mobility anisotropy is measured for transport both parallel and perpendicular to the polymer chain direction. The mobility anisotropy is relatively small, with the mobility along the polymer chain direction being higher by a factor of 3–5, consistent with the grain size encountered in the two transport directions.     

All-organic vertical transistor in an analogous n-semiconductor/metal/p-semiconductor trilayer structure

We report on the development and characterization of an all-organic vertical transistor, consisting of a p-type conjugated polymer, poly(bithiophene), as collector material, a poly(ethylene dioxythiophene)/poly(styrene sulfonate) layer as base material and a n-type molecule layer, Alq₃, as emitter material. The transistor is operated under direct bias in the common-emitter mode, being its operation based upon charge recombination of the injected majority carriers at the emitter–base interface. Experimental results have yielded current amplification factors up to 7. We also demonstrate that tunneling controls the transport characteristics of the device.     

High‐Sensitivity Floating‐Gate Phototransistors Based on WS2 and MoS2

In recent years, 2D layered materials have been considered as promising photon absorption channel media for next‐generation phototransistors due to their atomic thickness, easily tailored single‐crystal van der Waals heterostructures, ultrafast optoelectronic characteristics, and broadband photon absorption. However, the photosensitivity obtained from such devices, even under a large bias voltage, is still unsatisfactory until now. In this paper, high‐sensitivity phototransistors based on WS₂ and MoS₂ are proposed, designed, and fabricated with gold nanoparticles (AuNPs) embedded in the gate dielectric. These AuNPs, located between the tunneling and blocking dielectric, are found to enable efficient electron trapping in order to strongly suppress dark current. Ultralow dark current (10^?11 A), high photoresponsivity (1090 A W^?1), and high detectivity (3.5 × 10¹¹ Jones) are obtained for the WS₂ devices under a low source/drain and a zero gate voltage at a wavelength of 520 nm. These results demonstrate that the floating‐gate memory structure is an effective configuration to achieve high‐performance 2D electronic/optoelectronic devices.     

High‐Performance Nonvolatile Transistor Memories of Pentacence Using the Green Electrets of Sugar‐based Block Copolymers and Their Supramolecules

Reported here are the nonvolatile electrical characteristics of pentacene‐based organic field‐effect transistor (OFET) memory devices created from the green electrets of sugar‐based block copolymer maltoheptaose‐block‐polystyrene (MH‐b‐PS), and their supramolecules with 1‐aminopyrene (APy). The very hydrophilic and abundant‐hydroxyl MH block is employed as a charge‐trapping site, while the hydrophobic PS block serves as a matrix as well as a tunneling layer. The orientation of the MH nanodomains could be well controlled in the PS matrix with random spheres, vertical cylinders, and ordered horizontal cylinders via increasing solvent annealing time, leading to different electrical switching characteristics. The electron‐trapping ability induced by the horizontal‐cylinder MH is stronger than those of the random‐sphere and vertical‐cylinder structures, attributed to the effective contact area. The electrical memory window of the device is further improved via the supramolecules of hydrogen‐bonding 1‐aminopyrene to the MH moieties of MH‐b‐PS for enhancing the hole‐trapping ability. The optimized device using the horizontal cylinders of the supramolecule electret exhibits the excellent memory characteristics of a wide memory window (52.7 V), retention time longer than 10⁴ s with a high ON/OFF ratio of >10⁵, and stable reversibility over 200 cycles. This study reveals a new approach to achieve a high‐performance flash memory through the morphology control of sugar‐based block copolymers and their supramolecules.     

High Carrier Density and Metallic Conductivity in Poly(3‐hexylthiophene) Achieved by Electrostatic Charge Injection

The use of electrostatic charge injection (i.e., the transverse field effect) to induce both very large two‐dimensional hole densities (～ 10¹⁵ charges cm^–2) and metallic conductivities in poly(3‐hexylthiophene) (P3HT) is reported. Films of P3HT are electrostatically gated by a solution‐deposited polymer‐electrolyte gate dielectric in a field‐effect‐transistor configuration. Exceptionally high hole field‐effect mobilities (up to 0.7 cm² V^–1 s^–1) are measured concurrently with large hole densities, resulting in an extremely large sheet conductance of 200 μS sq.^–1. The large room‐temperature conductivity of 1000 S cm^–1 together with the very low measured activation energies (0.7–4 meV) suggest that the metal–insulator transition in P3HT is achieved. A maximum in sheet conductance versus charge density is also observed, which may result from near‐filling of the valence band or from charge correlations that lower the carrier mobility. Importantly, the large hole densities in P3HT are achieved using capacitive coupling between the polymer‐electrolyte gate dielectric and P3HT (i.e., the field effect) and not via chemical or electrochemical doping. Electrostatic control of carrier density up to 10¹⁵ charges cm^–2 (～ 10²² charges cm^–3) opens opportunities to explore systematically the importance of charge‐correlation effects on transport in conjugated polymers without the structural rearrangement associated with chemical or electrochemical doping.     

Hybrids of Magnetic Nanoparticles with Double‐Hydrophilic Core/Shell Cylindrical Polymer Brushes and Their Alignment in a Magnetic Field

The synthesis of double‐hydrophilic core/shell cylindrical polymer brushes (CPBs), their hybrids with magnetite nanoparticles, and the directed alignment of these magnetic hybrid cylinders by a magnetic field are demonstrated. Consecutive grafting from a polyinitiator poly(2‐(2‐bromoisobutyryloxy)ethyl methacrylate) (PBIEM) of tert‐butyl methacrylate (tBMA) and oligo(ethylene glycol) methacrylate (OEGMA) using atom‐transfer radical polymerization (ATRP) and further de‐protection yields core/shell CPBs with poly(methacrylic acid) (PMAA) as the core and POEGMA as the shell, which is evidenced by ¹H NMR, gel permeation chromatography (GPC), and dynamic and static light scattering (DLS and SLS). The resulting core/shell brush is well soluble in water and shows a pH responsiveness because of its weak polyelectrolyte core. Pearl‐necklace structures are observed by cryogenic transmission electron microscopy (cryo‐TEM) at pH 4, while at pH 7, these structures disappear owing to the ionization of the core. A similar morphology is also found for the polychelate of the core/shell CPBs with Fe³⁺ ions. Superparamagnetic magnetite nanoparticles have also been prepared and introduced into the core of the brushes. The hybrid material retains the superparamagnetic property of the magnetite nanoparticles, which is verified by superconducting quantum interference device (SQUID) magnetization measurements. Large‐scale alignment of the hybrid cylinders in relatively low magnetic fields (40–300 mT) can easily be performed when deposited on a surface. which is clearly revealed by the atomic force microscopy (AFM) and TEM measurements.     

Low‐Power Nonvolatile Charge Storage Memory Based on MoS2 and an Ultrathin Polymer Tunneling Dielectric

Low‐power, nonvolatile memory is an essential electronic component to store and process the unprecedented data flood arising from the oncoming Internet of Things era. Molybdenum disulfide (MoS₂) is a 2D material that is increasingly regarded as a promising semiconductor material in electronic device applications because of its unique physical characteristics. However, dielectric formation of an ultrathin low‐k tunneling on the dangling bond‐free surface of MoS₂ is a challenging task. Here, MoS₂‐based low‐power nonvolatile charge storage memory devices are reported with a poly(1,3,5‐trimethyl‐1,3,5‐trivinyl cyclotrisiloxane) (pV3D3) tunneling dielectric layer formed via a solvent‐free initiated chemical vapor deposition (iCVD) process. The surface‐growing polymerization and low‐temperature nature of the iCVD process enable the conformal growing of low‐k (≈2.2) pV3D3 insulating films on MoS₂. The fabricated memory devices exhibit a tunable memory window with high on/off ratio (≈10⁶), excellent retention times of 10⁵ s with an extrapolated time of possibly years, and an excellent cycling endurance of more than 10³ cycles, which are much higher than those reported previously for MoS₂‐based memory devices. By leveraging the inherent flexibility of both MoS₂ and polymer dielectric films, this research presents an important milestone in the development of low‐power flexible nonvolatile memory devices.