Room‐Temperature Printing of Organic Thin‐Film Transistors with π‐Junction Gold Nanoparticles

Printing semiconductor devices under ambient atmospheric conditions is a promising method for the large‐area, low‐cost fabrication of flexible electronic products. However, processes conducted at temperatures greater than 150 °C are typically used for printed electronics, which prevents the use of common flexible substrates because of the distortion caused by heat. The present report describes a method for the room‐temperature printing of electronics, which allows thin‐film electronic devices to be printed at room temperature without the application of heat. The development of π‐junction gold nanoparticles as the electrode material permits the room‐temperature deposition of a conductive metal layer. Room‐temperature patterning methods are also developed for the Au ink electrodes and an active organic semiconductor layer, which enables the fabrication of organic thin‐film transistors through room‐temperature printing. The transistor devices printed at room temperature exhibit average field‐effect mobilities of 7.9 and 2.5 cm² V^?1 s^?1 on plastic and paper substrates, respectively. These results suggest that this fabrication method is very promising as a core technology for low‐cost and high‐performance printed electronics.     

“Regioselective Deposition” Method to Pattern Silver Electrodes Facilely and Efficiently with High Resolution: Towards All‐Solution‐Processed,High‐Performance,Bottom‐Contacted,Flexible, Polymer‐Based Electronics

“Regioselectivity deposition” method is developed to pattern silver electrodes facilely and efficiently by solution‐process with high resolution (down to 2 μm) on different substrates in A4 paper size. With the help of this method, large‐area, flexible, high‐performance polymer field‐effect transistors based on the silver electrodes and polyimide insulator are fabricated with bottom‐contact configuration by all‐solution processes. The polymer devices exhibit high performance with average field‐effect mobility over 1.0 cm² V^?1 s^?1 (the highest mobility up to 1.5 cm² V^?1 s^?1) and excellent environmental stability and flexibility, indicating the cost effectiveness of this method for practical applications in organic electronics.     

Liquid‐Gated Transistors Based on Reduced Graphene Oxide for Flexible and Wearable Electronics

Graphene is regarded as the ultimate material for future flexible, high‐performance, and wearable electronics. Herein, a novel, robust, all‐green, highly reliable (yield ≥ 99%), and upscalable technology is reported for wearable applications comprising reduced graphene oxide (rGO) as the electroactive component in liquid‐gated transistors (LGTs). rGO is a formidable material for future flexible and wearable applications due to its easy processability, excellent surface reactivity, and large‐area coverage. A novel protocol is established toward the high‐yield fabrication of flexible rGO LGTs combining high robustness (>1.5 h of continuous operation) with state‐of‐the‐art performances, being similar to those of their rigid counterparts operated under liquid gating, including field‐effect mobility of ≈10^?1 cm² V^?1 s^?1 and transconductance of ≈25 µS. Permeable membranes have been proven crucial to operate flexible LGTs under mechanical stress with reduced amounts of solution (<20 µL). Our rGO LGTs are operated in artificial sweat exploiting two different layouts based on lateral‐flow paper fluidics. These approaches pave the road toward future real‐time tracking of perspiration via a simple and cost‐effective approach. The reported findings contribute to the robust and scalable production of novel graphene‐based flexible devices, whose features fulfill the requirements of wearable electronics.     

Seriography‐Guided Reduction of Graphene Oxide Biopapers for Wearable Sensory Electronics

Novel nacre‐mimic bio‐nanocomposites, such as graphene‐based laminates, are pushing the boundaries of strength and toughness as flexible engineering materials. Translating these material advances to functional flexible electronics requires methods for generating print‐scalable microcircuits (conductive elements surrounded by dielectric) into these strong, tough, lightweight bio‐nanocomposites. Here, a new paradigm for printing flexible electronics by employing facile, eco‐friendly seriography to confine the reduction of graphene oxide biopapers reinforced by silk interlayers is presented. Well‐defined, micropatterned regions on the biopaper are chemically reduced, generating a 10⁶ increase in conductivity (up to 10⁴ S m^?1). Flexible, robust graphene‐silk circuits are showcased in diverse applications such as resistive moisture sensors and capacitive proximity sensors. Unlike conductive (i.e., graphene‐ or Ag nanoparticle‐loaded) inks printed onto substrates, seriography‐guided reduction does not create mechanically weak interfaces between dissimilar materials and does not require the judicious formation of ink. The unimpaired functionality of printed‐in graphene‐silk microcircuits after thousands of punitive folding cycles and chemical attack by harsh solvents is demonstrated. This novel approach provides a low‐cost, portable solution for printing micrometer‐scale conductive features uniformly across large areas (>hundreds of cm²) in layered composites for applications including wearable health monitors, electronic skin, rollable antennas, and conformable displays.     

Reusable Cellulose‐Based Hydrogel Sticker Film Applied as Gate Dielectric in Paper Electrolyte‐Gated Transistors

A new concept for reusable eco‐friendly hydrogel electrolytes based on cellulose is introduced. The reported electrolytes are designed and engineered through a simple, fast, low‐cost, and eco‐friendly dissolution method of microcrystalline cellulose at low temperature using an aqueous LiOH/urea solvent system. The cellulose solution is combined with carboxymethyl cellulose, followed by the regeneration and simultaneous ion incorporation. The produced free standing cellulose‐based electrolyte films exhibit interesting properties for application in flexible electrochemical devices, such as biosensors or electrolyte‐gated transistors (EGTs), because of their high specific capacitances (4–5 µF cm^?2), transparency, and flexibility. Indium–gallium–zinc‐oxide EGTs on glass with laminated cellulose‐based hydrogel electrolytes (CHEs) as the gate dielectric are produced presenting a low working voltage (<2 V), showing an on–off current ratio (I _on/off) of 10⁶, a subthreshold swing lower than 0.2 V dec^?1, and saturation mobility (μ_Sat) reaching 26 cm² V^?1 s^?1. The flexible CHE‐gated transistors on paper are also demonstrated, which operate at switching frequencies up to 100 Hz. Combining the flexibility of the EGTs on paper with the reusability of the developed CHEs is a breakthrough toward biodegradable advanced functional materials allied with disposable/recyclable and low‐cost electronic devices.     

Inkjet Printing of Self‐Assembled 2D Titanium Carbide and Protein Electrodes for Stimuli‐Responsive Electromagnetic Shielding

2D titanium carbides (MXene) possess significant characteristics including high conductivity and electromagnetic interference shielding efficiency (EMI SE) that are important for applications in printed and flexible electronics. However, MXene‐based ink formulations are yet to be demonstrated for proper inkjet printing of MXene patterns. Here, tandem repeat synthetic proteins based on squid ring teeth (SRT) are employed as templates of molecular self‐assembly to engineer MXene inks that can be printed as stimuli‐responsive electrodes on various substrates including cellulose paper, glass, and flexible polyethylene terephthalate (PET). MXene electrodes printed on PET substrates are able to display electrical conductivity values as high as 1080 ± 175 S cm^?1, which significantly exceeds electrical conductivity values of state‐of‐the‐art inkjet‐printed electrodes composed of other 2D materials including graphene (250 S cm^?1) and reduced graphene oxide (340 S cm^?1). Furthermore, this high electrical conductivity is sustained under excessive bending deformation. These flexible electrodes also exhibit effective EMI SE values reaching 50 dB at films with thicknesses of 1.35 µm, which mainly originate from their high electrical conductivity and layered structure.     

Inkjet Printed Large‐Area Flexible Few‐Layer Graphene Thermoelectrics

Graphene‐based organic nanocomposites have ascended as promising candidates for thermoelectric energy conversion. In order to adopt existing scalable printing methods for developing thermostable graphene‐based thermoelectric devices, optimization of both the material ink and the thermoelectric properties of the resulting films are required. Here, inkjet‐printed large‐area flexible graphene thin films with outstanding thermoelectric properties are reported. The thermal and electronic transport properties of the films reveal the so‐called phonon‐glass electron‐crystal character (i.e., electrical transport behavior akin to that of few‐layer graphene flakes with quenched thermal transport arising from the disordered nanoporous structure). As a result, the all‐graphene films show a room‐temperature thermoelectric power factor of 18.7 µW m^?1 K^?2, representing over a threefold improvement to previous solution‐processed all‐graphene structures. The demonstration of inkjet‐printed thermoelectric devices underscores the potential for future flexible, scalable, and low‐cost thermoelectric applications, such as harvesting energy from body heat in wearable applications.     

High‐Performance Flexible Multilayer MoS2 Transistors on Solution‐Based Polyimide Substrates

Transition metal dichalcogenides (TMDs) layers of molecular thickness, in particular molybdenum disulfide (MoS₂), become increasingly important as active elements for mechanically flexible/stretchable electronics owing to their relatively high carrier mobility, wide bandgap, and mechanical flexibility. Although the superior electronic properties of TMD transistors are usually integrated into rigid silicon wafers or glass substrates, the achievement of similar device performance on flexible substrates remains quite a challenge. The present work successfully addresses this challenge by a novel process architecture consisting of a solution‐based polyimide (PI) flexible substrate in which laser‐welded silver nanowires are embedded, a hybrid organic/inorganic gate insulator, and multilayers of MoS₂. Transistors fabricated according to this process scheme have decent properties: a field‐effect‐mobility as high as 141 cm² V^?1 s^?1 and an I_on/I_off ratio as high as 5 × 10⁵. Furthermore, no apparent degradation in the device properties is observed under systematic cyclic bending tests with bending radii of 10 and 5 mm. Overall electrical and mechanical results provide potentially important applications in the fabrication of versatile areas of flexible integrated circuitry.     

Screen‐Printed Poly(3,4‐Ethylenedioxythiophene):Poly(Styrenesulfonate) Grids as ITO‐Free Anodes for Flexible Organic Light‐Emitting Diodes

Poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT: PSS) grids have been successfully constructed by roll‐to‐roll compatible screen‐printing techniques and have been used as indium tin oxide (ITO)‐free anodes for flexible organic light‐emitting diodes (OLEDs). The grid‐type transparent conductive electrodes (TCEs) can adopt thicker PEDOT: PSS grid lines to ensure the conductivity, while the mesh‐like grid structure can play an important role to maintain high optical transparency. By adjusting grid periods, grid thickness and treatment of organic additives, PEDOT: PSS TCEs with high optical transparency, low sheet resistance, and excellent mechanical flexibility have been achieved. Using the screen‐printed PEDOT: PSS grids as the anodes, ITO‐free OLEDs achieved peak current efficiency of 3.40 cd A^?1 at the current density of 10 mA cm^?2, which are 1.56 times better than the devices with ITO glass as the anodes. The improved efficiency is attributed to the light extraction effect and improved transparency by the grid structure. The superior optoelectronic performances of OLEDs based on flexible screen‐printed PEDOT: PSS grid anodes suggest their great prospects as ITO‐free anodes for flexible and wearable electronic applications.     

All‐Printed Porous Carbon Film for Electricity Generation from Evaporation‐Driven Water Flow

Converting environmental “waste energies” into electricity via a natural process is an ideal strategy for environmental energy harvesting and supplying power for distributed energy‐consuming devices. This paper reports that evaporation‐driven water flow within an all‐printed porous carbon film can reliably generate sustainable voltage up to 1 V with a power density of ≈8.1 µW cm^?3 under ambient conditions. The output performance of the device can be easily scaled up and used to power low‐power consumption electronic devices or for energy storage. Furthermore, the device is successfully used without electric storage as a direct power source for electrodeposition of silver microstructures. Because of the ubiquity of water evaporation in nature and the low cost of materials involved, the study presents a novel avenue to harvest ambient energy and has potential applications in low‐cost, green, self‐powered devices and systems.     

Solution‐Processable,High‐Performance Flexible Electroluminescent Devices Based on High‐k Nanodielectrics

Flexible alternating‐current electroluminescent (ACEL) devices have attracted considerable attention for their ability to produce uniform light emission under bent conditions and have enormous potential for applications in back lighting panels, decorative lighting in automobiles, and panel displays. Nevertheless, flexible ACEL devices generally require a high operating bias, which precludes their implementation in low power devices. Herein, solution‐processed La‐doped barium titanate (BTO:La) nanocuboids (≈150 nm) are presented as high dielectric constant (high‐k) nanodielectrics, which can enhance the dielectric constant of an ACEL device from 2.6 to 21 (at 1 kHz), enabling the fabrication of high‐performance flexible ACEL devices with a lower operating voltage as well as higher brightness (≈57.54 cd m^?2 at 240 V, 1 kHz) than devices using undoped BTO nanodielectrics (≈14.3 cd m^?2 at 240 V, 1 kHz). Furthermore, a uniform brightness across the whole panel surface of the flexible ACEL devices and excellent device reliability are achieved via the use of uniform networks of crossaligned silver nanowires as highly conductive and flexible electrodes. The results offer experimental validation of high‐brightness flexible ACELs using solution‐processed BTO:La nanodielectrics, which constitutes an important milestone toward the implementation of high‐k nanodielectrics in flexible displays.     

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.     

A Room‐Temperature High‐Conductivity Metal Printing Paradigm with Visible‐Light Projection Lithography

Fabricating electronic devices require integrating metallic conductors and polymeric insulators in complex structures. Current metal‐patterning methods such as evaporation and laser sintering require vacuum, multistep processes, and high temperature during sintering or postannealing to achieve desirable electrical conductivity, which damages low‐temperature polymer substrates. Here reports a facile ecofriendly room‐temperature metal printing paradigm using visible‐light projection lithography. With a particle‐free reactive silver ink, photoinduced redox reaction occurs to form metallic silver within designed illuminated regions through a digital mask on substrate with insignificant temperature change (<4 °C). The patterns exhibit remarkably high conductivity achievable at room temperature (2.4 × 10⁷ S m^?1, ≈40% of bulk silver conductivity) after simple room‐temperature chemical annealing for 1–2 s. The finest silver trace produced reaches 15 µm. Neither extra thermal energy input nor physical mask is required for the entire fabrication process. Metal patterns were printed on various substrates, including polyethylene terephthalate, polydimethylsiloxane, polyimide, Scotch tape, print paper, Si wafer, glass coverslip, and polystyrene. By changing inks, this paradigm can be extended to print various metals and metal–polymer hybrid structures. This method greatly simplifies the metal‐patterning process and expands printability and substrate materials, showing huge potential in fabricating microelectronics with one system.     

React‐on‐Demand (RoD) Fabrication of Highly Conductive Metal–Polymer Hybrid Structure for Flexible Electronics via One‐Step Direct Writing or Printing

As a fast prototyping technique, direct writing of flexible electronics is gaining popularity for its low‐cost, simplicity, ultrahigh portability, and ease of use. However, the latest handwritten circuits reported either have relative low conductivity or require additional post‐treatment, keeping this emerging technology away from end‐users. Here, a one‐step react‐on‐demand (RoD) method for fabricating flexible circuits with ultralow sheet resistance, enhanced safety, and durability is proposed. With the special functionalized substrate, a real‐time 3D synthesis of silver plates in microscale is triggered on‐demand right beneath the tip in the water‐swelled polyvinyl alcohol (PVA) coating, forming a 3D metal–polymer hybrid structure of ≈7 µm with one single stroke. The as‐fabricated silver traces show an enhanced durability and ultralow sheet resistance down to 4 mΩ sq^?1 which is by far the lowest sheet resistance reported in literatures achieved by direct writing. Meanwhile, PVA seal small particles inside the film, adding additional safety to this technology. Since neither nanomaterials nor a harsh fabrication environment are required, the proposed method remains low cost, user friendly, and accessible to end users. With little effort, the RoD approach can be extended to various printing systems, offering a particle‐free, sintering‐free solution for high‐resolution, high‐speed production of flexible electronics.     

Printed Sub‐2 V Gel‐Electrolyte‐Gated Polymer Transistors and Circuits

The fabrication and characterization of printed ion‐gel‐gated poly(3‐hexylthiophene) (P3HT) transistors and integrated circuits is reported, with emphasis on demonstrating both function and performance at supply voltages below 2 V. The key to achieving fast sub‐2 V operation is an unusual gel electrolyte based on an ionic liquid and a gelating block copolymer. This gel electrolyte serves as the gate dielectric and has both a short polarization response time (<1 ms) and a large specific capacitance (>10 µF cm^?2), which leads simultaneously to high output conductance (>2 mS mm^?1), low threshold voltage (<1 V) and high inverter switching frequencies (1–10 kHz). Aerosol‐jet‐printed inverters, ring oscillators, NAND gates, and flip‐flop circuits are demonstrated. The five‐stage ring oscillator operates at frequencies up to 150 Hz, corresponding to a propagation delay of 0.7 ms per stage. These printed gel electrolyte gated circuits compare favorably with other reported printed circuits that often require much larger operating voltages. Materials factors influencing the performance of the devices are discussed.     

All‐Carbon‐Electrode‐Based Endurable Flexible Perovskite Solar Cells

Endured, low‐cost, and high‐performance flexible perovskite solar cells (PSCs) featuring lightweight and mechanical flexibility have attracted tremendous attention for portable power source applications. However, flexible PSCs typically use expensive and fragile indium–tin oxide as transparent anode and high‐vacuum processed noble metal as cathode, resulting in dramatic performance degradation after continuous bending or thermal stress. Here, all‐carbon‐electrode‐based flexible PSCs are fabricated employing graphene as transparent anode and carbon nanotubes as cathode. All‐carbon‐electrode‐based flexible devices with and without spiro‐OMeTAD (2,2′,7,7′‐tetrakis‐(N,N‐di‐p‐methoxyphenylamine)‐9,9′‐spirobifluorene) hole conductor achieve power conversion efficiencies (PCEs) of 11.9% and 8.4%, respectively. The flexible carbon‐electrode‐based solar cells demonstrate superior robustness against mechanical deformation in comparison with their counterparts fabricated on flexible indium–tin oxide substrates. Moreover, all carbon‐electrode‐based flexible PSCs also show significantly enhanced stability compared to the flexible devices with gold and silver cathodes under continuous light soaking or 60 °C thermal stress in air, retaining over 90% of their original PCEs after 1000 h. The promising durability and stability highlight that flexible PSCs are fully compatible with carbon materials and pave the way toward the realization of rollable and low‐cost flexible perovskite photovoltaic devices.     

Impact of Morphology on Printed Contact Performance in Carbon Nanotube Thin‐Film Transistors

Silver nanoparticles (NPs) are the most widely used conductive material throughout the printed electronics space due to their high conductivity and low cost. However, when interfacing with other prominent printed materials, such as semiconducting carbon nanotubes (CNTs) in thin‐film transistors (TFTs), silver is suboptimal when compared to more expensive or less conductive materials. Consequently, there would be significant value to improving the interface of printed silver to CNT films. In this work, the impact of nanostructure morphology on the electrical properties of printed silver and nanotube junctions in CNT‐TFTs is investigated. Three distinct silver morphologies (NPs, nanoflakes – NFs, and nanowires – NWs) are explored with top‐ and bottom‐contact configurations for each. The NF morphology in a top‐contact configuration is found to yield the best electrical interface to CNTs, resulting in an average contact resistance of 1.2 MΩ ? µm. Beyond electrical performance, several trade‐offs in morphology selection are revealed, including print resolution and process temperature. While NF inks produce the best interfaces, NP inks produce the smallest features, and NW inks are compatible with low processing temperatures (<80 °C). These results outline the trade‐offs between silver contact morphologies in CNT‐TFTs and show that contact morphology selection can be tailored for specific applications.     

A Review of Low‐Temperature Solution‐Processed Metal Oxide Thin‐Film Transistors for Flexible Electronics

Solution processing, including printing technology, is a promising technique for oxide thin‐film transistor (TFTs) fabrication because it tends to be a cost‐effective process with high composition controllability and high throughput. However, solution‐processed oxide TFTs are limited by low‐performance and stability issues, which require high‐temperature annealing. This high thermal budget in the fabrication process inhibits oxide TFTs from being applied to flexible electronics. There have been numerous attempts to promote the desired electrical characteristics of solution‐processed oxide TFTs at lower fabrication temperatures. Recent techniques for achieving low‐temperature (<350 °C) solution‐processed and printed oxide TFTs, in terms of the materials, processes, and structural engineering methods currently in use are reviewed. Moreover, the core techniques for both n‐type and p‐type oxide‐based channel layers, gate dielectric layers, and electrode layers in oxide TFTs are addressed. Finally, various multifunctional and emerging applications based on low‐temperature solution‐processed oxide TFTs are introduced and future outlooks for this highly promising research are suggested.     

Scalable Production of Graphene Inks via Wet‐Jet Milling Exfoliation for Screen‐Printed Micro‐Supercapacitors

The miniaturization of energy storage units is pivotal for the development of next‐generation portable electronic devices. Micro‐supercapacitors (MSCs) hold great potential to work as on‐chip micro‐power sources and energy storage units complementing batteries and energy harvester systems. Scalable production of supercapacitor materials with cost‐effective and high‐throughput processing methods is crucial for the widespread application of MSCs. Here, wet‐jet milling exfoliation of graphite is reported to scale up the production of graphene as a supercapacitor material. The formulation of aqueous/alcohol‐based graphene inks allows metal‐free, flexible MSCs to be screen‐printed. These MSCs exhibit areal capacitance (C_areal) values up to 1.324 mF cm^?2 (5.296 mF cm^?2 for a single electrode), corresponding to an outstanding volumetric capacitance (C_vol) of 0.490 F cm^?3 (1.961 F cm^?3 for a single electrode). The screen‐printed MSCs can operate up to a power density above 20 mW cm^?2 at an energy density of 0.064 µWh cm^?2. The devices exhibit excellent cycling stability over charge–discharge cycling (10 000 cycles), bending cycling (100 cycles at a bending radius of 1 cm) and folding (up to angles of 180°). Moreover, ethylene vinyl acetate‐encapsulated MSCs retain their electrochemical properties after a home‐laundry cycle, providing waterproof and washable properties for prospective application in wearable electronics.     

Highly Conductive,Flexible, Polyurethane‐Based Adhesives for Flexible and Printed Electronics

Flexible interconnects are one of the key elements in realizing next‐generation flexible electronics. While wire bonding interconnection materials are being deployed and discussed widely, adhesives to support flip‐chip and surface‐mount interconnections are less commonly used and reported. A polyurethane (PU)‐based electrically conductive adhesive (ECA) is developed to meet all the requirements of flexible interconnects, including an ultralow bulk resistivity of ≈1.0 × 10^?5 Ω cm that is maintained during bending, rolling, and compressing, good adhesion to various flexible substrates, and facile processing. The PU‐ECA enables various interconnection techniques in flexible and printed electronics: it can serve as a die‐attach material for flip‐chip, as vertical interconnect access (VIA)‐filling and polymer bump materials for 3D integration, and as a conductive paste for wearable radio‐frequency devices.