Flexible, Low-Power Thin-Film Transistors Made of Vapor-Phase Synthesized High‑<i>k</i>, Ultrathin Polymer Gate Dielectrics

A series of high-<i>k</i>, ultrathin copolymer gate dielectrics were synthesized from 2-cyanoethyl acrylate (CEA) and di­(ethylene glycol) divinyl ether (DEGDVE) monomers by a free radical polymerization via a one-step, vapor-phase, initiated chemical vapor deposition (iCVD) method. The chemical composition of the copolymers was systematically optimized by tuning the input ratio of the vaporized CEA and DEGDVE monomers to achieve a high dielectric constant (<i>k</i>) as well as excellent dielectric strength. Interestingly, DEGDVE was nonhomopolymerizable but it was able to form a copolymer with other kinds of monomers. Utilizing this interesting property of the DEGDVE cross-linker, the dielectric constant of the copolymer film could be maximized with minimum incorporation of the cross-linker moiety. To our knowledge, this is the first report on the synthesis of a cyanide-containing polymer in the vapor phase, where a high-purity polymer film with a maximized dielectric constant was achieved. The dielectric film with the optimized composition showed a dielectric constant greater than 6 and extremely low leakage current densities (<3 × 10^–8 A/cm² in the range of ±2 MV/cm), with a thickness of only 20 nm, which is an outstanding thickness for down-scalable cyanide polymer dielectrics. With this high-<i>k</i> dielectric layer, organic thin-film transistors (OTFTs) and oxide TFTs were fabricated, which showed hysteresis-free transfer characteristics with an operating voltage of less than 3 V. Furthermore, the flexible OTFTs retained their low gate leakage current and ideal TFT characteristics even under 2% applied tensile strain, which makes them some of the most flexible OTFTs reported to date. We believe that these ultrathin, high-<i>k</i> organic dielectric films with excellent mechanical flexibility will play a crucial role in future soft electronics

Direct Observation of a Carbon Filament in Water-Resistant Organic Memory

The memory for the Internet of Things (IoT) requires versatile characteristics such as flexibility, wearability, and stability in outdoor environments. Resistive random access memory (RRAM) to harness a simple structure and organic material with good flexibility can be an attractive candidate for IoT memory. However, its solution-oriented process and unclear switching mechanism are critical problems. Here we demonstrate iCVD polymer-intercalated RRAM (i-RRAM). i-RRAM exhibits robust flexibility and versatile wearability on any substrate. Stable operation of i-RRAM, even in water, is demonstrated, which is the first experimental presentation of water-resistant organic memory without any waterproof protection package. Moreover, the direct observation of a carbon filament is also reported for the first time using transmission electron microscopy, which puts an end to the controversy surrounding the switching mechanism. Therefore, reproducibility is feasible through comprehensive modeling. Furthermore, a carbon filament is superior to a metal filament in terms of the design window and selection of the electrode material. These results suggest an alternative to solve the critical issues of organic RRAM and an optimized memory type suitable for the IoT era

Flexible Nonvolatile Polymer Memory Array on Plastic Substrate via Initiated Chemical Vapor Deposition

Resistive random access memory based on polymer thin films has been developed as a promising flexible nonvolatile memory for flexible electronic systems. Memory plays an important role in all modern electronic systems for data storage, processing, and communication; thus, the development of flexible memory is essential for the realization of flexible electronics. However, the existing solution-processed, polymer-based RRAMs have exhibited serious drawbacks in terms of the uniformity, electrical stability, and long-term stability of the polymer thin films. Here, we present poly­(1,3,5-trimethyl-1,3,5-trivinyl cyclotrisiloxane) (pV3D3)-based RRAM arrays fabricated via the solvent-free technique called initiated chemical vapor deposition (iCVD) process for flexible memory application. Because of the outstanding chemical stability of pV3D3 films, the pV3D3-RRAM arrays can be fabricated by a conventional photolithography process. The pV3D3-RRAM on flexible substrates showed unipolar resistive switching memory with an on/off ratio of over 10⁷, stable retention time for 10⁵ s, excellent cycling endurance over 10⁵ cycles, and robust immunity to mechanical stress. In addition, pV3D3-RRAMs showed good uniformity in terms of device-to-device distribution. The pV3D3-RRAM will pave the way for development of next-generation flexible nonvolatile memory devices

Photolithography-Based Patterning of Liquid Metal Interconnects for Monolithically Integrated Stretchable Circuits

We demonstrate a new patterning technique for gallium-based liquid metals on flat substrates, which can provide both high pattern resolution (∼20 μm) and alignment precision as required for highly integrated circuits. In a very similar manner as in the patterning of solid metal films by photolithography and lift-off processes, the liquid metal layer painted over the whole substrate area can be selectively removed by dissolving the underlying photoresist layer, leaving behind robust liquid patterns as defined by the photolithography. This quick and simple method makes it possible to integrate fine-scale interconnects with preformed devices precisely, which is indispensable for realizing monolithically integrated stretchable circuits. As a way for constructing stretchable integrated circuits, we propose a hybrid configuration composed of rigid device regions and liquid interconnects, which is constructed on a rigid substrate first but highly stretchable after being transferred onto an elastomeric substrate. This new method can be useful in various applications requiring both high-resolution and precisely aligned patterning of gallium-based liquid metals