Hyejeong Seong

Synthesis of ultrathin polymer insulating layers by initiated chemical vapour deposition for low-power soft electronics

Insulating layers based on oxides and nitrides provide high capacitance, low leakage, high breakdown field and resistance to electrical stresses when used in electronic devices based on rigid substrates. However, their typically high process temperatures and brittleness make it difficult to achieve similar performance in flexible or organic electronics. Here, we show that poly(1,3,5-trimethyl-1,3,5-trivinyl cyclotrisiloxane) (pV3D3) prepared via a one-step, solvent-free technique called initiated chemical vapour deposition (iCVD) is a versatile polymeric insulating layer that meets a wide range of requirements for next-generation electronic devices. Highly uniform and pure ultrathin films of pV3D3 with excellent insulating properties, a large energy gap (>8 eV), tunnelling-limited leakage characteristics and resistance to a tensile strain of up to 4% are demonstrated. The low process temperature, surface-growth character, and solvent-free nature of the iCVD process enable pV3D3 to be grown conformally on plastic substrates to yield flexible field-effect transistors as well as on a variety of channel layers, including organics, oxides, and graphene.

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.

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.

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 10(7), stable retention time for 10(5) s, excellent cycling endurance over 10(5) 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.

Logic circuits composed of flexible carbon nanotube thin-film transistor and ultra-thin polymer gate dielectric.

Printing electronics has become increasingly prominent in the field of electronic engineering because this method is highly efficient at producing flexible, low-cost and large-scale thin-film transistors. However, TFTs are typically constructed with rigid insulating layers consisting of oxides and nitrides that are brittle and require high processing temperatures, which can cause a number of problems when used in printed flexible TFTs. In this study, we address these issues and demonstrate a method of producing inkjet-printed TFTs that include an ultra-thin polymeric dielectric layer produced by initiated chemical vapor deposition (iCVD) at room temperature and highly purified 99.9% semiconducting carbon nanotubes. Our integrated approach enables the production of flexible logic circuits consisting of CNT-TFTs on a polyethersulfone (PES) substrate that have a high mobility (up to 9.76 cm2 V−1 sec−1), a low operating voltage (less than 4 V), a high current on/off ratio (3 × 104), and a total device yield of 90%. Thus, it should be emphasized that this study delineates a guideline for the feasibility of producing flexible CNT-TFT logic circuits with high performance based on a low-cost and simple fabrication process.

Foldable and Disposable Memory on Paper

Foldable organic memory on cellulose nanofibril paper with bendable and rollable characteristics is demonstrated by employing initiated chemical vapor deposition (iCVD) for polymerization of the resistive switching layer and inkjet printing of the electrode, where iCVD based on all-dry and room temperature process is very suitable for paper electronics. This memory exhibits a low operation voltage of 1.5 V enabling battery operation compared to previous reports and wide memory window. The memory performance is maintained after folding tests, showing high endurance. Furthermore, the quick and complete disposable nature demonstrated here is attractive for security applications. This work provides an effective platform for green, foldable and disposable electronics based on low cost and versatile materials.

Ultra-low power, highly uniform polymer memory by inserted multilayer graphene electrode

Filament type resistive random access memory (RRAM) based on polymer thin films is a promising device for next generation, flexible nonvolatile memory. However, the resistive switching nonuniformity and the high power consumption found in the general filament type RRAM devices present critical issues for practical memory applications. Here, we introduce a novel approach not only to reduce the power consumption but also to improve the resistive switching uniformity in RRAM devices based on poly(1,3,5-trimethyl-3,4,5-trivinyl cyclotrisiloxane) by inserting multilayer graphene (MLG) at the electrode/polymer interface. The resistive switching uniformity was thereby significantly improved, and the power consumption was markedly reduced by 250 times. Furthermore, the inserted MLG film enabled a transition of the resistive switching operation from unipolar resistive switching to bipolar resistive switching and induced self-compliance behavior. The findings of this study can pave the way toward a new area of application for graphene in electronic devices.

Organic flash memory on various flexible substrates for foldable and disposable electronics

With the emergence of wearable or disposable electronics, there grows a demand for a flash memory realizable on various flexible substrates. Nevertheless, it has been challenging to develop a flash memory that simultaneously exhibits a significant level of flexibility and performance. This is mainly due to the scarcity of flexible dielectric materials with insulating properties sufficient for a flash memory, which involves dual dielectric layers, respectively, responsible for tunneling and blocking of charges. Here we report ultra-flexible organic flash memories based on polymer dielectrics prepared by initiated chemical vapor deposition. Using their near-ideal dielectric characteristics, we demonstrate flash memories bendable down to a radius of 300 μm that exhibits a relatively long-projected retention with a programming voltage on par with the present industrial standards. The proposed memory technology is then applied to non-conventional substrates, such as papers, to demonstrate its feasibility in a wide range of applications.Flexible flash memory is crucial to modern electronics, but its fabrication is challenging in the absence of suitable dielectric materials. Here, Lee et al. realize organic memory with retention over 10 years using tunneling and blocking dielectric layers prepared by initiated chemical vapor deposition.

Zero-static-power nonvolatile logic-in-memory circuits for flexible electronics

Flexible logic circuits and memory with ultra-low static power consumption are in great demand for battery-powered flexible electronic systems. Here, we show that a flexible nonvolatile logic-in-memory circuit enabling normally-off computing can be implemented using a poly(1,3,5-trivinyl-1,3,5-trimethyl cyclotrisiloxane) (pV3D3)-based memristor array. Although memristive logic-in-memory circuits have been previously reported, the requirements of additional components and the large variation of memristors have limited demonstrations to simple gates within a few operation cycles on rigid substrates only. Using memristor-aided logic (MAGIC) architecture requiring only memristors and pV3D3-memristor with good uniformity on a flexible substrate, for the first time, we experimentally demonstrated our implementation of MAGIC-NOT and -NOR gates during multiple cycles and even under bent conditions. Other functions, such as OR, AND, NAND, and a half adder, are also realized by combinations of NOT and NOR gates within a crossbar array. This research advances the development of novel computing architecture with zero static power consumption for batterypowered flexible electronic systems.

Site-specific immobilization of proteins on non-conventional substrates via solvent-free initiated chemical vapour deposition (iCVD) process

Currently, the development of protein chips faces new requirements of improved environmental stability, disposability, and cost-effectiveness for their wide applicability in our daily life. Here, we demonstrate a new protein detection platform on low-cost plastic and paper substrates. To achieve this platform, a highly selective thiol–ene photochemical reaction between vinyl functionality on the surface and cysteine-linked protein was utilized to immobilize the relevant proteins on the disposable substrates. First, the surface of the flexible substrates was modified with a vinyl-containing polymer, poly(2,4,6,8-tetravinyl-2,4,6,8-tetramethyl cyclotetrasiloxane) (pV4D4), via a solvent-free initiated chemical vapour deposition (iCVD) process. Next, on the vinyl functionalized surface, cysteine-linked proteins were covalently immobilized by a UV-assisted thiol–ene click reaction. The solvent-free characteristic of iCVD enabled us to directly pattern the functionality on the substrate via shadow mask patterning. On the patterned substrate, selective immobilization of the proteins was possible. With four model proteins, including two fluorescent proteins, single-chain variable fragment (scFv), and non-immunoglobulin protein scaffold (human kringle domain), we successfully demonstrated the immobilization of proteins on various substrates including polyethylene (PE) film and chromatography paper.