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This work demonstrates sensitive and low-cost piezoelectric sensors on skin-friendly, ultrathin, and conformable substrates combined with organic electrochemical transistors (OECTs) for the detection and amplification of alternating low-voltage input signals. The fully screen-printed (SP) piezoelectric sensors were manufactured on commercially available tattoo paper substrates, while the all-printed OECTs, relying on an extended gate electrode architecture, were manufactured either by solely using SP or by combining SP and aerosol jet printing (AJP) on PET substrates. Applying a low-voltage signal (±25 mV) to the gate electrode of the SP+AJP OECT results in approximately five times higher current modulation as compared to the fully SP reference OECT. The tattoo paper-based substrate enables transfer of the SP piezoelectric sensor to the skin, which in turn allows for radial pulse monitoring when combined with the SP+AJP OECT; this is possible due to the ability of the conformable sensor to convert mechanical vibrations into voltage signals along with the highly sensitive current modulation ability of the transistor device to further amplify the output signal. The results reported herein pave the way toward all-printed fully conformable wearable devices with high sensitivity to be further utilized for the real-time monitoring of electrophysiological signals.

Large area electronics (LAE) with the capability to sense and retain information are crucial for advances in applications such as wearables, digital healthcare, and robotics. The big data generated by these sensor-laden systems need to be scaled down or processed locally. In this regard, brain-inspired computing and in-memory computing have attracted considerable interest. However, suitable architectures have mainly been developed using costly and resource-intensive conventional lithography-based methods. There is a need for the development of innovative, resource-efficient fabrication routes that enable such devices and concepts. Herein, we present ZnO nanowire (NW)-based memristors on a polyimide substrate fabricated by a LAE-compatible and resource-efficient route comprising solution processing and printing technologies. High-resolution "drop-on-demand" and "direct ink write" printers are employed to deposit metallic layers (silver and gold) and a ZnO seed layer, needed for the site-selective growth of ZnO NWs via a low-cost hydrothermal method. The printed memristors show high bipolar resistance switching (ON/OFF ratio >10 3 ) between two nonvolatile states and consistent switching at ultralow voltages (all devices showed switching at amplitudes <200 mV), with the best performing device showing consistent cycled resistance switching over 4 orders of magnitude with SET and RESET voltages of about 71 and -57 mV, respectively. Thus, the presented devices offer reliable high resistance switching at the lowest reported voltage for printed memristors and prove to be competitive with many conventional nanofabrication-based devices. The presented results show the potential printed memristors technology holds for large-area, low-voltage sensing applications such as electronic skin.

The absence of scalable and environmentally sustainable methods for producing electronic-grade graphene nanoplatelets remains a barrier to the industrial-scale application of graphene in printed electronics and conductive composites. To address this unmet need, here we report the utilization of carboxylated cellulose nanocrystals (CNCs) extracted from the perennial tall grass Miscanthus × giganteus as a biorenewable dispersant for the aqueous liquid-phase exfoliation of few-layer graphene nanoplatelets. This CNC-based exfoliation procedure was optimized using a Bayesian machine learning model, resulting in a significant graphite-to-graphene conversion yield of 13.4% and a percolating graphene thin-film electrical conductivity of 3.4 × 10 4 S m -1 . The as-exfoliated graphene dispersions were directly formulated into an aerosol jet printing ink using cellulose-based additives to achieve high-resolution printing (∼20 μm line width). Life cycle assessment of this CNC-based exfoliation method showed substantial improvements for fossil fuel consumption, greenhouse gas emissions, and water consumption compared to incumbent liquid-phase exfoliation methods for electronic-grade graphene nanoplatelets. Mechanistically, potential mean force calculations from molecular dynamics simulations reveal that the high exfoliation yield can be traced back to the favorable surface interactions between CNCs and graphene. Ultimately, the use of biorenewable CNCs for liquid-phase exfoliation will accelerate the scalable and eco-friendly manufacturing of graphene for electronically conductive applications.

In recent years, significant advancements in printed electronics and flexible materials have catalyzed the development of electronic skins for wearable applications. However, the low glass transition temperature of flexible substrates poses a challenge as it is incompatible with the high-temperature annealing required for electrode fabrication, thereby limiting the performance of flexible electronic devices. In this study, we address these limitations by proposing a novel flexible device manufacturing process that combines adhesive printing patterning with a transfer printing technology. By employing poly(vinylidene fluoride) (PVDF)/graphene nitride (GCN) as the transfer substrate and dielectric layer, we successfully fabricated a high-performance dual-mode touch sensor on a large scale. The successful development of this dual-mode sensor can be attributed to two key factors: the construction of a robust hydrogen-bonding network between the PVDF/GCN dielectric layer and the carbon electrode and the ability of GCN to restrict the movement of PVDF molecular chains within the dielectric layer. This restriction reduces the overall polarization of the film, enabling the formation of a complete device structure with a highly sensitive edge electric field. The noncontact sensors developed in this study are fully printable into sensor arrays and can be seamlessly integrated with internet of things technology for wearable applications. These sensors exhibit exceptional tactile response and facilitate effective human-machine interactions over extended distances, underscoring their significant potential in fields such as healthcare and artificial intelligence.

The miniaturization and widespread deployment of electronic devices across diverse environments have heightened their vulnerability to corrosion, particularly affecting copper traces within printed circuit boards (PCBs). Conventional protective methods, such as conformal coatings, face challenges including the necessity for a critical thickness to ensure effective barrier properties and the requirement for multiple steps of drying and curing to eliminate solvent entrapment within polymer coatings. This study investigates cold atmospheric plasma (CAP) as an innovative technique for directly depositing ultrathin silicon oxide (SiO x ) coatings onto copper surfaces to enhance corrosion protection in PCBs. A systematic investigation was undertaken to examine how the scanning speed of the CAP deposition head impacts the film quality and corrosion resistance. The research aims to determine the optimal scanning speed of the CAP deposition head that achieves complete surface coverage while promoting effective cross-linking and minimizing unreacted precursor entrapment, resulting in superior electrical barrier and mechanical properties. The CAP coating process demonstrated the capability of depositing SiO x onto copper surfaces at various thicknesses ranging from 70 to 1110 nm through a single deposition process by simply adjusting the scanning speed of the plasma head (5-75 mm/s). Evaluation of material corrosion barrier characteristics revealed that scanning speeds of 45 mm/s of the plasma deposition head provided an effective coating thickness of 140 nm, exhibiting superior corrosion resistance (30-fold) compared to that of uncoated copper. As a proof of concept, the efficacy of CAP-deposited SiO x coatings was demonstrated by protecting an LED circuit in saltwater and by coating printed circuits for potential agricultural sensor applications. These CAP-deposited coatings offer performance comparable to or superior to traditional conformal polymeric coatings. This research presents CAP-deposited SiO x coatings as a promising approach for effective and scalable corrosion protection in miniaturized electronics.

Additive manufacturing (AM) is emerging as an eco-friendly method for minimizing waste, as the demand for responsive materials in IoT and Industry 4.0 is on the rise. Magnetoactive composites, which are manufactured through AM, facilitate nonintrusive remote sensing and actuation. Printed magnetoelectric composites are an innovative method that utilizes the synergies between magnetic and electric properties. The study of magnetoelectric effects, including the recently validated piezoinductive effect, demonstrates the generation of electric voltage through external AC and DC magnetic fields. This shift in magnetic sensors, utilizing piezoinductive effect of the piezoelectric polymer poly(vinylidene fluoride), PVDF, eliminates the need for magnetic fillers in printed devices, aligning with sustainability principles, essential for the deployment of IoT and Industry 4.0. The achieved sensitivity surpasses other studies by 100 times, showcasing linear outputs for both applied AC and DC magnetic fields. Additionally, the sensor capitalizes on the linear phase shift of the generated signal with an applied DC magnetic field, an unprecedented effect. Thus, this work introduces a remarkable magnetoactive device with a sensitivity of S T = 95.1 ± 0.9 μV Oe -1 mT -1 , a significantly improved performance compared to magnetoelectric devices using polymer composites. As a functional proof of concept of the developed system, a magnetic position sensor has been demonstrated.

Two-dimensional (2D) semiconductor field-effect film transistors combine large carrier mobility with mechanical flexibility and therefore can be ideally suitable for wearable electronics or at the sensor interfaces of smart sensor systems. However, such applications require large-area solution processing as opposed to single-flake devices, where the critical challenge to overcome is the high interflake resistance values. In this report, using a narrow-channel, near-vertical transport device architecture, we have fabricated inkjet-printed sub-20 nm channel electrolyte-gated transistors with predominantly intraflake carrier transport. Therefore, the electronics transport in these transistors is not dominated by the high interflake resistance, and the intraflake material properties including doping density, defect concentration, contact resistance, and threshold voltage modulation can be examined and optimized independently to achieve a current density as high as 280 μA·μm -1 . In addition, through the passivation of the sulfur vacancies with a tailored surface treatment, we demonstrate an impressive On-Off current ratio exceeding 1 × 10 7 , complemented by a low subthreshold swing of 100 mV·decade -1 . Next, exploiting these high-performance transistors, unipolar depletion-load-type inverters have been fabricated that show a maximum gain of 31. Furthermore, we have realized NAND, NOR, and OR gates, demonstrating their seamless operation at a frequency of 1 kHz. Therefore, this work represents an important step forward to realize electronic circuits based on printed 2D thin film transistors.

It is critical to understand molecular ordering processes in small-molecule organic semiconductor (OSC) films in optimizing electronic device applications, although it is difficult to observe and investigate the ordering characteristics at a mesoscopic or device scale. Here, we report that friction force microscopy (FFM) allows visualizing the ordering transformation process from a thermodynamically metastable phase to a stable phase at a mesoscopic scale. We utilized 2-octyl-benzothieno[3,2- b ]naphtho[2,3- b ]thiophene (2-C8-BTNT) as a typical highly layered-crystalline OSC. We found that the friction force between an AFM tip and spin-coated OSC films significantly depends on whether local film states are in metastable monolayer phase or stable bilayer-type herringbone (b-LHB) phase that exhibits high carrier mobility. The formation of the stable b-LHB phase leads to lower friction than the metastable monolayer phase, clearly visualizing the molecular order. Force map (Fmap) analysis indicates that the lower friction in the b-LHB phase should be associated with the reduction of interfacial adhesion force. Notably, the observed results demonstrate that the spin-coated thin film changes from continuous film with the monolayer phase to rugged microcrystal grains with the b-LHB phase when left at ambient conditions. By contrast, an appropriate post-thermal annealing process facilitates the phase transformation without inducing such morphological changes. The technique provides a unique and effective tool for revealing the relationship between processing conditions and device performance in polycrystalline OSC films.

The switching of conventional field-effect transistors (FETs) is limited by the Boltzmann barrier of thermionic emission, which prevents the realization of low-power electronics. In order to overcome this limitation, among others, unconventional device geometry with a ferroelectric/dielectric insulator stack has been proposed to demonstrate stable negative-capacitance behavior. Here, the switching of the ferroelectric layer behaves like a step-up amplifier and results in a body factor less than 1. This implies a larger change in the semiconductor surface potential compared to the applied gate voltage variation. The transistors with such ferroelectric/dielectric stack are known as negative-capacitance field-effect transistors (nc-FETs), and can demonstrate a subthreshold slope lower than the Boltzmann's limit (60 mV/decade). While nc-FETs have typically been realized with high-vacuum-deposition processes, here we show fully printed nc-FETs with amorphous indium-gallium-zinc oxide (a-IGZO) as the semiconductor material, Al 2 O 3 as the dielectric, and poly(vinylidene fluoride-trifluoroethylene) (PVDF-TrFE) as the polymer ferroelectric. The printed nc-FETs demonstrate an extremely low subthreshold slope of ∼2.3 mV/decade at room temperature, which remains below the Boltzmann's limit for over 5 orders of magnitude of drain currents. Furthermore, the unipolar depletion-load-type inverters fabricated using n-type nc-FETs have demonstrated an extraordinary signal gain of 2691.

Hybrid core-shell nanoparticles with metal cores and conductive polymer shells yield materials that are sinter-free and highly conductive but mechanically weak. Conventional composites of such nanoparticles are electrically insulating. Here, we introduce microscale phase-separated nanocomposites of hybrid gold-PEDOT:PPS particles in insulating poly(vinyl alcohol) (PVA). They combine electrical conductivities of up to 2.1 × 10 5 S/m at 10 vol % PVA with increased mechanical adhesion on polyethylene terephthalate and glass substrates. We studied the effects of the PVA molecular weight, hydrolyzation degree, and volume fraction. Composites with 10 vol % highly hydrolyzed PVA at a M W of 89-98 kDa had the highest conductivities and stabilities; highly hydrolyzed PVA even increased the conductivity of the hybrid particle layers. We propose the formation of hydrogen bonds between PVA and PEDOT:PSS that lead to demixing and the formation of stable, structured composites. Finally, we demonstrated the inkjet-printability of inks containing PVA in water with viscosities of 1.6-2.0 Pa s at 50.1 s -1 and prepared bending-resistant electrical leads.

Additive manufacturing holds promise for rapid prototyping and low-cost production of biosensors for diverse pathogens. Among additive manufacturing methods, screen printing is particularly desirable for high-throughput production of sensing platforms. However, this technique needs to be combined with carefully formulated inks, rapid postprocessing, and selective functionalization to meet all requirements for high-performance biosensing applications. Here, we present screen-printed graphene electrodes that are processed with thermal annealing to achieve high surface area and electrical conductivity for sensitive biodetection via electrochemical impedance spectroscopy. As a proof-of-concept, this biosensing platform is utilized for electrochemical detection of SARS-CoV-2. To ensure reliable specificity in the presence of multiple variants, biolayer interferometry (BLI) is used as a label-free and dynamic screening method to identify optimal antibodies for concurrent affinity to the Spike S1 proteins of Delta, Omicron, and Wild Type SARS-CoV-2 variants while maintaining low affinity to competing pathogens such as Influenza H1N1. The BLI-identified antibodies are robustly bound to the graphene electrode surface via oxygen moieties that are introduced during the thermal annealing process. The resulting electrochemical immunosensors achieve superior metrics including rapid detection (55 s readout following 15 min of incubation), low limits of detection (approaching 500 ag/mL for the Omicron variant), and high selectivity toward multiple variants. Importantly, the sensors perform well on clinical saliva samples detecting as few as 10 3 copies/mL of SARS-CoV-2 Omicron, following CDC protocols. The combination of the screen-printed graphene sensing platform and effective antibody selection using BLI can be generalized to a wide range of point-of-care immunosensors.

This article introduces a methodology to increase the integration density of functional electronic features on fibers/threads/wires through additive deposition of functional materials via printed electronics. It opens the possibility to create a multifunctional intelligent system on a single fiber/thread/wire while combining the advantages of existing approaches, i.e., the scalability of coating techniques and the microfeatures of semiconductor-based fabrication. By directly printing on threads (of diameters ranging from 90 to 1000 μm), micropatterned electronic devices and multifunctional electronic systems could be formed. Contact and noncontact printing methods were utilized to create various shapes from serpentines and meanders to planar coils and interdigitated electrodes, as well as complex multilayer structures for thermal and light actuators, humidity, and temperature sensors. We demonstrate the practicality of the method by integrating a multifunctional thread into a FFP mask for breath monitoring. Printing technologies provide virtually unrestricted choices for the types of threads, materials, and devices used. They are scalable via roll-to-roll processes and offer a resource-efficient way to democratize electronics across textile products.

Multimaterial aerosol jet printing offers a unique capability to freely mix inks with different chemical compositions in the aerosol phase, enabling one-step digital fabrication with tailored compositions or functionally graded structures, including in the x-y plane. Here, in situ mixing of two carbon nanomaterial inks with distinct electrical properties is demonstrated. By tailoring the mixing ratio of the constituent inks, electrical conductivity is modulated by 130×, and sheet resistance values for a single pass span approximately 2 orders of magnitude. The ability to manufacture components with tailored electrical properties offers significant value for hybrid and flexible electronic device applications, such as microelectronics packaging. Moreover, grading properties within a part provides a new dimension of design freedom for complex assemblies.

The proliferation of printed electronic devices is feeding the growth of the Internet of Things, with devices deployed everywhere to collect and communicate data. At the same time, the increase in low-cost disposable devices is a cause for serious environmental concern. In particular, widely used plastic substrates such as poly(ethylene terephthalate) are persistent hazards to the environment. Paper is promising as a greener substrate for printed electronics because it is biodegradable and sourced from renewable materials as well as being low cost and compatible with roll-to-roll printing. However, the porous microstructure of paper promotes wicking of functional inks, leading to poor electrical performance and printing resolution. Hydrophobic coatings applied to the surface of paper create a planarized, printable surface, but these materials may compromise biodegradability and/or recyclability. This paper describes a new resist-free patterning method for printed paper-based electronics that takes advantage of the porous structure of paper. Debossed contact printing uses the pressure from a debossing tip to compress the porous structure of paper and create a patterned relief structure. Printing functional inks with an unpatterned roller deposits ink only on the raised regions of the relief structure. We demonstrate debossed contact printing of silver, carbon black, and conducting polymer inks and show that this new fabrication method is suitable for the fabrication of printed devices with dense features. We demonstrate the fabrication of antennas and patterned electrodes for RFID and smart wallpaper applications, respectively.

Transparent conductors (TCs) represent key components in many applications from optoelectronic devices to electromagnetic shielding. While commercial applications typically use thin films of indium tin oxide, this material is brittle and increasingly scarce, meaning higher performing and cheaper alternatives are sought after. Solution-processible metals would be ideal owing to their high conductivities and printability. However, due to their opacity to visible light, such films need to be very thin to achieve transparency, thus limiting the minimum resistance achievable. One solution is to print metallic particles in a grid structure, which has the advantages of high tunable transparency and resistance at the cost of uniformity. Here, we report silver nanosheets that have been aerosol jet printed into grids as high-performance transparent conductors. We first investigate the effect of annealing on the silver nanosheets where we observe the onset of junction sintering at 160 °C after which the silver network becomes continuous. We then investigate the effect of line width and thickness on the electrical performance and the effect of varying the aperture dimensions on the optical performance. Using these data, we develop simple models, which allow us to optimize the grid and demonstrate a printed transparent conductor with a transmittance of 91% at a sheet resistance of 4.6 Ω/sq.

Direct write printing is restricted by the lack of dielectric materials that can be printed with high resolution and offer dissipation factors at radio frequency (RF) within the range of commercial RF laminates. Herein, we outline the development of dielectric materials with dielectric loss below 0.006 in X and Ku frequency bands (8.2-18 GHz), the range required for radio frequency and microwave applications. The described materials were designed for printability and processability, specifically a prolonged viscosity below 1000 cps and a robust cure procedure, which requires minimal heat treatment. In the first stage of this work, nonpolar ring-opening metathesis polymerization (ROMP) is demonstrated at room temperature in an open-air environment with a low-viscosity monomer, 5-vinyl-2-norbornene, using the second-generation Grubbs catalyst (G-II). Differential scanning calorimetry (DSC) was used to study how the catalyst activity is increased with heating at various stages in the reaction, which is then used as a strategy to cure the material after printing. The resulting cured poly(5-vinyl-2-norbornene) material is then characterized for dielectric and mechanical performance before and after a secondary heat treatment, which mimics processing procedures to incorporate subsequent printed conductor layers for multilayer applications. After the secondary heat treatment, the material exhibits a 55.0% reduction in the coefficient of thermal expansion (CTE), an increase in glass-transition temperature ( T g ) from 32.4 to 46.1 °C, and an increased 25 °C storage modulus from 428 to 1031 MPa while demonstrating a minimal change in dielectric loss. Lastly, samples of the developed dielectric material are printed with silver overtop to demonstrate how the material can be effectively incorporated into fully printed, multilayer RF applications.

Wearable electronics is an emerging field in academics and industry, in which electronic devices, such as smartwatches and sensors, are printed or embedded within textiles. The electrical circuits in electronics textile (e-textile) should withstand many cycles of bending and stretching. Direct printing of conductive inks enables the patterning of electrical circuits; however, while using conventional nanoparticle-based inks, printing onto the fabric results in a thin layer of a conductor, which is not sufficiently robust and impairs the reliability required for practical applications. Here, we present a new process for fabricating robust stretchable e-textile using a thermodynamically stable, solution-based copper complex ink, which is capable of full penetrating the fabric. After printing on knitted stretchable fabrics, they were heated, and the complex underwent an intermolecular self-reduction reaction. The continuously formed metallic copper was used as a seed layer for electroless plating (EP) to form highly conductive circuits. It was found that the stretching direction has a significant role in resistivity. This new approach enables fabricating e-textiles with high stretchability and durability, as demonstrated for wearable gloves, toward printing functional e-textile.

High-throughput production methods such as screen printing can bring stretchable electronics out of the lab into the market. Most stretchable conductor inks for screen printing are based on silver nanoparticles or flakes due to their favorable performance-to-cost ratio, but silver is prone to tarnishing and corrosion, thereby limiting the stability of such conductors. Here, we report on a cost-efficient and scalable approach to resolve this issue by developing screen printable inks based on silver flakes chemically coated by a thin layer of gold. The printed stretchable AgAu conductors reach a conductivity of 8500 S cm -1 , remain conductive up to 250% strain, show excellent corrosion and tarnishing stability, and are used to demonstrate wearable LED and NFC circuits. The reported approach is attractive for smart clothing, as the long-term functionality of such devices is expected in a variety of environments.

Printing technologies are changing the face of electronics with features such as resource-efficiency, low-cost, and novel form factors. While significant advances have been made in terms of organic electronics, the high-performance and stable transistors by printing, and their large-scale integration leading to fast integrated circuits remains a major challenge. This is because of the difficulties to print high-mobility semiconducting materials and the lack of high-resolution printing techniques. Herein, we present silicon based printed n- and p-channel transistors to demonstrate the possibility of developing high-performance complementary metal-oxide-semiconductor (CMOS) computing architecture. The direct roll transfer printing is used here for deterministic assembly of high-mobility single crystal silicon nanoribbons arrays on a flexible polyimide substrate. This is followed by high-resolution electrohydrodynamic printing to define source/drain/gate electrodes and to encapsulate, thus leading to printed devices. The printed transistors show effective peak mobilities of 15 cm 2 /(V s) (n-channel) and 5 cm 2 /(V s) (p-channel) at low 1 V drain bias. Furthermore, the effect of electrical, mechanical, and thermal stress on the performance and stability of the encapsulated transistors is investigated. The transistors showed stable transfer characteristics even after: (i) continuous 4000 transfer cycles, (ii) excruciating 10000 bending cycles at different bending radii (40, 25, and 15 mm), and (iii) between 15 and 60 °C temperatures.

Printing technologies are gaining growing attention as a sustainable route for the fabrication of high-performance and flexible power sources such as microsupercapacitors (MSCs). Here, the inkjet printing method is utilized for the fabrication of manganese dioxide (MnO 2 )-based, flexible all-solid-state MSCs on surface-modified A4 paper substrate. The appropriate rheology of the formulated ethanol-based ink (Fromm number <10) and the proper dimensions of MnO 2 nanoflowers (average size ∼600 nm) ensure a reliable inkjet printing process. Moreover, the underlying graphene/Ag nanowire pattern serves as a primer and highly conductive ( R s < 2 Ω sq -1 ) layer on top of the paper to facilitate the anchoring of MnO 2 nanoflowers and rapid electron transportation. The resulting all-solid-state MSCs deliver a maximum areal capacitance of 0.68 mF cm -2 at a current density of 25 μA cm -2 , reasonable durability (>80% of capacity remained after 3000 cycles), and remarkable foldability. Additionally, the inkjet-printed MSC devices deliver a superior areal energy density of 0.01 μWh cm -2 and also a power density of 1.19 μW cm -2 . This study demonstrates the power of the inkjet printing method to produce MSCs on flexible substrates, which have great potential for flexible/wearable electronics.

Aerosol jet printing is a noncontact, digital, additive manufacturing technique compatible with a wide variety of functional materials. Although promising, development of new materials and devices using this technique remains hindered by limited rational ink formulation, with most recent studies focused on device demonstration rather than foundational process science. In the present work, a systematic approach to formulating a polymer-stabilized graphene ink is reported, which considers the effect of solvent composition on dispersion, rheology, wetting, drying, and phase separation characteristics that drive process outcomes. It was found that a four-component solvent mixture composed of isobutyl acetate, diglyme, dihydrolevoglucosenone, and glycerol supported efficient ink atomization and controlled in-line drying to reduce overspray and wetting instabilities while maintaining high resolution and electrical conductivity, thus overcoming a trade-off in deposition rate and resolution common to aerosol jet printing. Biochemical sensors were printed for amperometric detection of the pesticide parathion, exhibiting a detection limit of 732 nM and a sensitivity of 34 nA μM -1 , demonstrating the viability of this graphene ink for fabricating functional electronic devices.

Biosensors based on miniaturized, functional electrodes are of high potential for various biosensing applications, especially at the point-of-care setting among others. However, the sensor performance of such electrochemical devices is still strongly limited, especially due to surface fouling in complex sample fluids, such as blood serum. Electrode coatings based on conductive nanomaterials embedded in antifouling matrices offer a promising strategy to overcome this limitation. However, known composite coatings require long (typically >24 h) and complex fabrication processes, which pose a strong barrier for cost-effective mass manufacturing and successful commercialization. Here, we describe a novel polymer/carbon nanotube (CNT) composite coating that can be produced from an ink containing a photoreactive and antifouling copolymer as well as conductive CNTs using fast and highly scalable printing processes. Coatings were prepared on screen-printed electrodes and characterized using cyclic voltammetry (CV) and protein fouling experiments. The coatings offered an electroactive surface area (EASA) comparable to uncoated screen-printed electrodes and retained >90% of initial EASA after 1 h of exposure to concentrated bovine serum albumin solution, while uncoated electrodes decreased to <20% of initial EASA after the same treatment. Utilizing the universal crosslinking reaction of the polymer coating, antibodies against the inflammatory biomarker C-reactive protein (CRP) were photochemically immobilized on the electrodes. Functionalized electrodes were fabricated in <2 h and were successfully used to quantify nanogram-range concentrations of CRP spiked in undiluted human blood serum using a sandwich-immunoassay with electrochemical read-out, demonstrating the high potential of the platform for biosensing applications.

Silver nanoparticles of average size 12-13 nm were successfully decorated on the surface of multiwalled carbon nanotubes (MWCNTs) through a scalable wet chemical method without altering the structure of the MWCNTs. Employing this Ag@MWCNT, a multifunctional room-temperature curable conductive ink was developed, with PEDOT:PSS as the conductive binder. Screen printing of the ink could yield conductive planar traces with a 9.5 μm thickness and a conductivity of 28.99 S/cm, minimal surface roughness, and good adhesion on Mylar and Kapton. The versatility of the ink for developing functional elements for printed electronics was demonstrated by fabricating prototypes of a wearable strain sensor, a smart glove, a wearable heater, and a wearable breath sensor. The printed strain sensor exhibited a massive sensing range for wearable applications, including an impressive 1332% normalized resistance change under a maximum stretchability of 23% with superior cyclic stability up to 10 000 cycles. The sensor also exhibited an impeccable gauge factor of 142 for a 5% strain (59 for 23%). Furthermore, the sensor was integrated into a smart glove that could flawlessly replicate a human finger's gestures with a minimal response time of 225-370 ms. Piezoresistive vibration sensors were also fabricated by printing the ink on Mylar, which was employed to fabricate a smart mask and a smart wearable patch to monitor variations in human respiratory and pulmonary cycles. Finally, an energy-efficient flexible heater was fabricated using the developed ink. The heater could generate a uniform temperature distribution of 130 °C at the expense of only 393 mW/cm 2 and require a minimum response time of 20 s. Thus, the unique formulation of Ag@MWCNT ink proved suitable for versatile devices for future wearable applications.

A flexible supercapacitor (SC) is an attractive energy storage device for powering low-power sensors, since it can be built using only nontoxic and sustainable materials. In this study, the advantages of using biodegradable polylactic acid (PLA) substrate for printed SC are investigated by studying the SC's cyclic bending reliability, failure mechanism, and the impact of the bending radius. The results confirm that the SCs with laminated PLA with polymer barrier substrate exhibited the highest bending reliability, stability, and capability in preventing liquid electrolyte evaporation among the investigated substrates. Besides, the reliability decreased with the decreasing bending radius only when the strongly impacted areas lie on the electrode, the flaking and cracking of which was found to be the failure mechanisms of the tested SCs, except for the SCs with PLA/Al substrate, which failed due to the Al cracking. This research suggests that using PLA/barrier substrate, developing more robust activated carbon electrodes, developing cellulose paper with more dense fiber structure and smaller porous areas, and controlling the bending radius are crucial to improving the SC's reliability.

Continuous conducting lines of width 5-20 μm have been printed with a Ag nanoparticle ink using drop-on-demand (DOD) electrohydrodynamic (EHD) inkjet printing on Si and PDMS substrates, with advancing contact angles of 11° and 35°, respectively, and a zero receding contact angle. It is only possible to achieve stable parallel sided lines within a limited range of drop spacings, and this limiting range for stable line printing decreases as the contact angle of the ink on the substrate increases. The upper bound drop spacing for stable line formation is determined by a minimum drop overlap required to prevent contact line retraction, and the lower bound is governed by competing flows for drop spreading onto an unwetted substrate and a return flow driven by a Laplace pressure difference between the newly deposited drops and the fluid some distance from the growing tip. The upper and lower bounds are shown to be consistent with those predicted using existing models for the stability of inkjet printed lines produced using piezoelectric droplet generators. A comparison with literature data for EHD printed lines finds that these limiting bounds apply with printed line widths as small as 200 nm using subfemtoliter drop volumes. When a fine grid pattern is printed, local differences in Laplace pressure lead to the line width retracting to the minimum stable width and excess ink being transported to the nodes of the grid. After printing and sintering, the printed tracks have a conductivity of about 15%-20% of bulk Ag on the Si substrate, which correlates with a porosity of about 60%.

Solution-based printing has contributed to the facile deposition of various types of materials, including the building blocks of printed electronics. In particular, solution-processable organic semiconductors (OSCs) are regarded as one of the most fascinating candidates for the fabrication of printed electronics. Herein, we report electrohydrodynamic (EHD) jet-printed p- and n-type OSCs, namely 6,13-bis(triisopropylsilylethynyl)pentacene (TIPS-PEN) and 6,13-bis((triisopropylsilyl)ethynyl)-5,7,12,14-tetraazapentacene (TIPS-TAP), and their use as single-OSC layers and as OSC mixed p-n layers to fabricate solution-processed p-, n-, and ambipolar-type organic field-effect transistors (OFETs). Use of the dragging mode of EHD jet printing, a process driven under a low electrostatic field with a short nozzle-to-substrate distance, was found to provide favorable conditions for growth of TIPS-PEN and TIPS-TAP crystals. In this way, the similar molecular structures of TIPS-PEN and TIPS-TAP yielded a homogeneous solid solution and showed ambipolar transport properties in OFETs. Therefore, the combination of single- and mixed-OSC layers enabled the preparation of various charge-transported devices from unit to integrated devices (NOT, NAND, NOR, and multivalued logic). Therefore, this fabrication technology can be useful for assisting in the production of OSC layers for practical applications in the near future.

There is growing interest in the development of novel materials and devices capable of ionizing radiation detection for medical applications. Organic semiconductors are promising candidates to meet the demands of modern detectors, such as low manufacturing costs, mechanical flexibility, and a response to radiation equivalent to human tissue. However, organic semiconductors have typically been employed in applications that convert low energy photons into high current densities, for example, solar cells and LEDs, and thus existing design rules must be re-explored for ionizing radiation detection where high energy photons are converted into typically much lower current densities. In this work, we report the optoelectronic and X-ray dosimetric response of a tissue equivalent organic photodetector fabricated with solution-based inks prepared from polymer donor poly(3-hexylthiophene) (P3HT) blended with either a non-fullerene acceptor (5 Z ,5' Z )-5,5'-((7,7'-(4,4,9,9-tetraoctyl-4,9-dihydro- s -indaceno[1,2- b :5,6- b ']dithiophene-2,7-diyl)bis(benzo[ c ][1,2,5]thiadiazole-7,4-diyl))bis(methanylylidene))bis(3-ethyl-2-thioxothiazolidin-4-one) ( o -IDTBR) or a fullerene acceptor, [6,6]-phenyl-C61-butyric acid methyl ester (PCBM). Indirect detection of X-rays was achieved via coupling of organic photodiodes with a plastic scintillator. Both detectors displayed an excellent response linearity with dose, with sensitivities to 6 MV photons of 263.4 ± 0.6 and 114.2 ± 0.7 pC/cGy recorded for P3HT:PCBM and P3HT:o-IDTBR detectors, respectively. Both detectors also exhibited a fast temporal response, able to resolve individual 3.6 μs pulses from the linear accelerator. Energy dependence measurements highlighted that the photodetectors were highly tissue equivalent, though an under-response in devices compared to water by up to a factor of 2.3 was found for photon energies of 30-200 keV due to the response of the plastic scintillator. The P3HT:o-IDTBR device exhibited a higher stability to radiation, showing just an 18.4% reduction in performance when exposed to radiation doses of up to 10 kGy. The reported devices provide a successful demonstration of stable, printable, flexible, and tissue-equivalent radiation detectors with energy dependence similar to other scintillator-based detectors used in radiotherapy.

Recently, machine learning has gained considerable attention in noncontact direct ink writing because of its novel process modeling and optimization techniques. Unlike conventional fabrication approaches, noncontact direct ink writing is an emerging 3D printing technology for directly fabricating low-cost and customized device applications. Despite possessing many advantages, the achieved electrical performance of produced microelectronics is still limited by the printing quality of the noncontact ink writing process. Therefore, there has been increasing interest in the machine learning for process optimization in the noncontact direct ink writing. Compared with traditional approaches, despite machine learning-based strategies having great potential for efficient process optimization, they are still limited to optimize a specific aspect of the printing process in the noncontact direct ink writing. Therefore, a systematic process optimization approach that integrates the advantages of state-of-the-art machine learning techniques is in demand to fully optimize the overall printing quality. In this paper, we systematically discuss the printing principles, key influencing factors, and main limitations of the noncontact direct ink writing technologies based on inkjet printing (IJP) and aerosol jet printing (AJP). The requirements for process optimization of the noncontact direct ink writing are classified into four main aspects. Then, traditional methods and the state-of-the-art machine learning-based strategies adopted in IJP and AJP for process optimization are reviewed and compared with pros and cons. Finally, to further develop a systematic machine learning approach for the process optimization, we highlight the major limitations, challenges, and future directions of the current machine learning applications.

We report on the fabrication and characterization of electronic devices printed with inks of quasi-one-dimensional (1D) van der Waals materials. The quasi-1D van der Waals materials are characterized by 1D motifs in their crystal structure, which allow for their exfoliation into bundles of atomic chains. The ink was prepared by the liquid-phase exfoliation of crystals of TiS 3 into quasi-1D nanoribbons dispersed in a mixture of ethanol and ethylene glycol. The temperature-dependent electrical measurements indicate that the electron transport in the printed devices is dominated by the electron hopping mechanisms. The low-frequency electronic noise in the printed devices is of 1/ f γ - nanoribbons as well as modifications in the hopping transport regime. The obtained results attest to the potential of quasi-1D van der Waals materials for applications in printed electronics.f is the frequency). The abrupt changes in the temperature dependence of the noise spectral density and γ parameter can be indicative of the phase transition in individual TiS 3 nanoribbons as well as modifications in the hopping transport regime. The obtained results attest to the potential of quasi-1D van der Waals materials for applications in printed electronics.

Flexible, lightweight, low-power, and low-cost displays are an active area of interest in the electronics community. In this work, we have developed a composite electrothermochromic material consisting of silver nanowires (Ag NWs) and thermochromic powders, which exhibits reversible color (phase) change during biasing due to Joule heating. A wide variety of color combinations are possible with suitable thermochromic material selection. We have formulated this composite material as a printable ink so that patterned deposition can be achieved in a single step. A low processing temperature of 100 °C makes the composite compatible with a wide range of flexible substrates such as paper and polyethylene terephthalate (PET). The material (encapsulated with polydimethylsiloxane (PDMS)) exhibits good flexibility and is observed to be functional after 10 000 bending cycles with <7% resistance change. We have fabricated a low-power seven-segment color display to show the material's suitability for practical display applications. We have also demonstrated that the same layer can function as a display and as a touch sensor because of its conducting and chromatic properties without additional active layers on top. The material is suitable for the fabrication of low-cost, flexible touch color displays for interactive electronic readers, digital posters, and flexible digital signboards.

Printed piezoresistive strain sensors based on stretchable roll-to-roll screen-printed silver electrodes on polydimethylsiloxane substrates and inkjet-deposited single-wall carbon nanotube micropatterns are demonstrated in this work. With the optimization of surface wetting and inkjet printing parameters, well-defined microscopic line patterns of the nanotubes with a sheet resistance of <100 Ω/□ could be deposited between stretchable Ag electrodes on the plasma-treated substrate. The developed stretchable devices are highly sensitive to tensile strain with a gauge factor of up to 400 and a pressure sensitivity of ∼0.09 Pa -1 , respond to bending down to a radius of 1.5 mm, and are suitable for mounting on the skin to monitor and resolve various movements of the human body such as cardiac cycle, breathing, and finger flexing. This study indicates that inkjet deposition of nanomaterials can complement well other printing technologies to produce flexible and stretchable devices in a versatile manner.

A stretchable conductor is one of the key components in soft electronics that allows the seamless integration of electronic devices and sensors on elastic substrates. Its unique advantages of mechanical flexibility and stretchability have enabled a variety of wearable bioelectronic devices that can conformably adapt to curved skin surfaces for long-term health monitoring applications. Here, we report a poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS)-based stretchable polymer blend that can be patterned using an inkjet printing process while exhibiting low sheet resistance and accommodating large mechanical deformations. We have systematically studied the effect of various types of polar solvent additives that can help induce phase separation of PEDOT and PSS grains and change the conformation of a PEDOT chain, thereby improving the electrical property of the film by facilitating charge hopping along the percolating PEDOT network. The optimal ink formulation is achieved by adding 5 wt % ethylene glycol into a pristine PEDOT:PSS aqueous solution, which results in a sheet resistance of as low as 58 Ω/□. Elasticity can also be achieved by blending the above solution with the soft polymer poly(ethylene oxide) (PEO). Thin films of PEDOT:PSS/PEO polymer blends patterned by inkjet printing exhibits a low sheet resistance of 84 Ω/□ and can resist up to 50% tensile strain with minimal changes in electrical performance. With its good conductivity and elasticity, we have further demonstrated the use of the polymer blend as stretchable interconnects and stretchable dry electrodes on a thin polydimethylsiloxane (PDMS) substrate for photoplethysmography (PPG) and electrocardiography (ECG) recording applications. This work shows the potential of using a printed stretchable conducting polymer in low-cost wearable sensor patches for smart health applications.

Recently, Ni and Ni-Cu nanoparticle-based inks have gained considerable research interest because of their high corrosion resistance as conductors in electronic devices. However, reported inks based on Cu-Ni nanoparticles need to be sintered at high temperatures above 300 °C to obtain electrodes with high conductivity on the order of 10 -5 Ω·cm. This study proposes a new conductive Cu-Ni-based hybrid ink that could be sintered at only 150-180 °C for producing Cu-Ni electrodes with low electrical resistance, high oxidation resistance, and flexibility. The hybrid ink contains Cu flakes and a complex of nickel formate and 1-amino-2-propanol (NiF-AmIP complex). At 150-180 °C, the Cu flakes catalyze the self-reduction of the NiF-AmIP complex, and Cu-Ni electrodes with high conductivity (on the order of 10 -5 Ω·cm) are formed on flexible polymer substrates at temperatures exceeding 150 °C. Analysis indicates that metallic Ni was decorated on the Cu flakes (especially on the edge) to improve the electrode's conductivity, oxidation resistance, and flexibility by forming bridging interconnections between the Cu flakes. The Cu-Ni electrodes demonstrated high stability against oxidation up to approximately 400 °C in air, as well as at 80 °C and 80% RH after 7 days. In addition to the excellent oxidation stability, the Cu-Ni electrode showed high durability under mechanical bending stress. Such sintered Cu-Ni electrodes obtained from hybrid inks have great potentials in printed/flexible devices due to their oxidation resistance and cost-effectiveness.

Eco-friendly and cost-effective materials and processes to manufacture functional substrates are crucial to further advance the area of printed electronics. One potential key component in the printed electronics platform is an electrically functionalized paper, produced by simply mixing common cellulosic pulp fibers with high-performance electroactive materials. Herein, an electronic paper including nanographite has been prepared using a standardized and scalable papermaking technique. No retention aid was needed to achieve a conducting nanographite loading as high as 50 wt %. The spontaneous retention that provides the integrity and stability of the nanographite paper, likely originates partially from an observed water-stable adhesion of nanographite flakes onto the fiber surfaces. The resulting paper exhibits excellent electrical characteristics, such as an in-plane conductivity of 107 S/cm and an areal capacitance of 9.2 mF/cm 2 , and was explored as the back-electrode in printed electrochromic displays.

X-ray tomographic reconstruction reveals that the distribution of Ag after inkjet printing and sintering a nanoparticle conducting ink on a woven polyester textile substrate is strongly controlled by the fiber surface properties and fabric architecture. Capillarity confines the transport of the ink predominantly within the warp or weft yarns of the fabric and there is little transport of ink between the yarns. Changing the fiber surface energy through the Scotchgard treatment leads to an increase in the contact angle, reducing ink transport along the fibers and an increase in conductance. A similar effect is seen when printed drop spacing is reduced, increasing the local Ag concentration. Electrical conductivity is strongly influenced by the fiber density in each yarn direction and, in this case, the different densities lead to different electrical conductance values. Through the use of image segmentation, it is possible to identify a low level of electrical interconnection between the warp and weft yarns. Conductance within a yarn is shown to depend on Ag concentration via a percolation mechanism and this is confirmed by a simple model relating the volume of the largest interconnected Ag object present to the measured conductance. These results illustrate the complexity of the interaction between conductive inks and fibrous substrates and that concepts, such as sheet resistance, used to characterize printed conductors on solid substrates are not applicable to textile substrates.

Semiconducting carbon nanotube (CNT) networks exhibit electrical, mechanical, and chemical properties attractive for thin-film applications, and printing allows for scalable and economically favorable fabrication of CNT thin-film transistors (TFTs). However, device-to-device variation of printed CNT-TFTs remains a concern, which largely stems from variations in printed CNT thin-film morphology and resulting properties. In this work, we overcome the challenges associated with printing uniformity and demonstrate an aerosol jet printing process that yields devices exhibiting a hole mobility of μ h = 12.5 cm 2 /V·s with a relative standard deviation as small as 4% (from over 38 devices). The enabling factors of such high uniformity include control of the CNT ink bath temperature during printing, ink formulation with nonvolatile and viscosifying additives, and a thermal treatment for polymer removal. It is discovered that a low CNT ink temperature benefits aerosol jet printing uniformity and stability in both short-term (∼1 min) and long-term (∼1 h) printing settings. These findings shed light on the effect of a commonly overlooked dimension of CNT aerosol jet printing and provide a practical strategy for large-scale, high-consistency realization of CNT-TFTs.

Increasing attention has been given to amine-copper formate complexes for their use as low-cost printable conductive inks. The structure of amine ligands coordinated to copper centers has been reported to dictate the properties of copper molecular inks, such as stability and printability, thereby influencing the copper reduction pathway during the thermolysis. Yet, the underlying mechanism by which formate is oxidized when complexed with amine ligands is still not fully understood. Here, we propose a mechanistic pathway of copper formate dehydrogenation and decarboxylation and examine the critical role that amine ligands play in their thermal decomposition by employing first-principles electronic structure computations and experimental analyses of thermolysis reactions. Based on the computational characterization of the relevant reaction pathways for a number of primary and secondary amines as well as pyridine ligand complexes, we are the first to show that the hydrogen bonds formed between the amine ligand and formate are the key factors governing the activation energy, providing a design principle for the synthesis of organic ligands that can tune the height of the reaction barriers of the dehydrogenation and decarboxylation reactions. The calculations, confirmed by NMR studies, show that the reduction of Cu(II) to Cu(I) occurs in concert with the release of H 2 via the dimerization of Cu(II) hydride. This result suggests that the monomeric elimination of H 2 is not favorable for the Cu(II) to Cu(I) reduction and thus identifies dimeric amino copper formate as an important intermediate for copper reduction whose thermodynamic stabilities are also dictated by the nature of the amine ligands.

Previous efforts to directly write conductive metals have been narrowly focused on nanoparticle ink suspensions that require aggressive sintering (>200 °C) and result in low-density, small-grained agglomerates with electrical conductivities <25% of bulk metal. Here, we demonstrate aerosol jet printing of a reactive ink solution and characterize high-density (93%) printed silver traces having near-bulk conductivity and grain sizes greater than the electron mean free path, while only requiring a low-temperature (80 °C) treatment. We have developed a predictive electronic transport model which correlates the microstructure to the measured conductivity and identifies a strategy to approach the practical conductivity limit for printed metals. Our analysis of how grain boundaries and tortuosity contribute to electrical resistivity provides insight into the basic materials science that governs how an ink formulator or process developer might approach improving the conductivity. Transmission line measurements validate that electrical properties are preserved up to 20 GHz, which demonstrates the utility of this technique for printed RF components. This work reveals a new method of producing robust printed electronics that retain the advantages of rapid prototyping and three-dimensional fabrication while achieving the performance necessary for success within the aerospace and communications industries.

Biodegradable electronics is a rapidly growing field, and the development of controllably biodegradable, high-conductivity materials suitable for additive manufacturing under ambient conditions remains a challenge. In this report, printable conductive pastes that employ poly(lactic acid) (PLA) as a binder and tungsten as a conductor are demonstrated. These composite conductors can provide enhanced stability in applications where moisture may be present, such as environmental monitoring or agriculture. Post-processing the printed traces using a solvent-aging technique increases their conductivity by up to 2 orders of magnitude, with final conductivities approaching 5000 S/m. Such techniques could prove useful when thermal processes including heating or laser sintering are limited by the temperature constraints of typical biodegradable substrates. Both accelerated oxidative and hydrolytic degradation of the printed composite conductors are examined, and a fully biodegradable capacitive soil moisture sensor is fabricated and tested.

In recent years, additive manufacturing of polydimethylsiloxane (PDMS) has gained interest for the development of soft electronics. To build complex electrical devices, fabrication of multilayered structures is required. We propose here a straightforward digital printing fabrication process of silicone rubber-based, multilayered electronics. An inkjet-printable PDMS solution was developed for the digital patterning of elastomeric structures. The silicone ink was used together with a highly conductive silver nanoparticle (Ag NP) ink for the fabrication of all-inkjet-printed multilayered electrical devices. The application of the multilayered circuit board was successful. The sheet resistances were below 0.3 Ω/□, and the conductive layer thickness was less than 1 μm. The electrical insulation between the conductive layers was done by printing a 20-25 μm-thick dielectric PDMS layer selectively on top of the bottommost conductive layer.

Graphene-based inks are becoming increasingly attractive for printing low-cost and flexible electrical circuits due to their high electrical conductivity, biocompatibility, and manufacturing scalability. Conventional graphene printing techniques, such as screen and inkjet printing, are limited by stringent ink viscosity requirements properties and large as-printed line width that impedes the performance of printed biosensors. Here, we report an aerosol-jet-printed (AJP) graphene-based immunosensor capable of monitoring two distinct cytokines: interferon gamma (IFN-γ) and interleukin 10 (IL-10). Interdigitated electrodes (IDEs) with 40 μm finger widths were printed from graphene-nitrocellulose ink on a polyimide substrate. The IDEs were annealed in CO 2 to introduce reactive oxygen species on the graphene surface that act as chemical handles to covalently link IFN-γ and IL-10 antibodies to the graphene surfaces. The resultant AJP electrochemical immunosensors are capable of monitoring cytokines in serum with wide sensing range (IFN-γ: 0.1-5 ng/mL; IL-10: 0.1-2 ng/mL), low detection limit (IFN-γ: 25 pg/ml and IL-10: 46 pg/ml) and high selectivity (antibodies exhibited minimal cross-reactivity with each other and IL-6) without the need for sample prelabeling or preconcentration. Moreover, these biosensors are mechanically flexible with minimal change in signal output after 250 bending cycles over a high curvature (Φ = 5 mm). Hence, this technology could be applied to numerous electrochemical applications that require low-cost electroactive circuits that are disposable and/or flexible.

Electrostatic force-assisted dispensing (EFAD)-printed tungsten trioxide (WO 3 )-based electrochromic devices (ECDs) displaying a dual image depending on the applied voltage are demonstrated. We first print WO 3 via EFAD printing, in which the width of the printed lines can be tuned by adjusting the printing speed. The performance of the ECDs is characterized while varying the thickness of the printed WO 3 film. It is determined that ∼550 nm thick WO 3 is the optimal film considering maximum transmittance contrast (Δ T max ), device dynamic responses, efficiency, and long-term coloration/bleaching cyclic stability. More significantly, the coloration of the devices in this work can alternatively appear due to the use of electrolyte-soluble anodic species (here, dimethyl ferrocene, dmFc), for which WO 3 ECDs alternately displaying a dual image, which is expected to have high potential as a functional component of printed electronics.3 ECDs alternately displaying a dual image, which is expected to have high potential as a functional component of printed electronics.

Slot die coating has been established as an economical approach for deposition of parallel narrow stripes, a constituent pattern feature in many printed device applications. However, the minimum feature size that can be achieved using this approach is constrained by wetting and liquid bridge phenomena at the deposition region. We hypothesize that pattern resolution and process control can be improved by co-depositing a support fluid to stabilize the pattern. Electrically conductive poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) is slot die-coated in parallel stripes on flexible poly(ethylene terephthalate) substrate, without wettability-enhancing dopants or substrate pretreatment. A miscible liquid phase, polyvinyl alcohol, is used as the support material. Feature size performance and conductivity of PEDOT:PSS stripe regions are evaluated across a range of process conditions. Narrow PEDOT:PSS stripes produced using our technique range from 400 to 850 μm and exhibit conductivity approaching 1.5 S cm -1 . This electrical performance falls within the upper range expected prior to standard conductivity-enhancing post-treatments. Significantly, dewetting effects normally present with undoped PEDOT:PSS on the plastic substrate are fully mitigated with our deposition technique. These results indicate high ease of processing and good feature size performance, with few inherent drawbacks to the functional properties of the patterned films.

Additive manufacturing has dramatically transformed the design and fabrication of advanced objects. Printed electronics-an additive thin-film processing technology-aims to realize low-cost, large-area electronics, and fabrication of devices with highly customized architectures. Recent advances in printing technology have led to several innovative applications; however, layer-on-layer deposition persists as a challenging issue. Here, the additive manufacturing of functional oxide devices by inkjet printing is presented. Two conditions appear critical for successful layer-on-layer printing: (i) preservation of stable surface properties and (ii) suppression of the material accumulation at the edges of a feature upon drying. The former condition was satisfied by introducing a surface modification layer of a polymer with nanotextured topography, and the latter was satisfied by designing the solvent composition of the ink. The developed process is highly efficient and enables conformal stacking of functional oxide layers according to the user-defined geometry, sequence arrangement, and layer thickness. To prove the effectiveness of this concept, we demonstrate an additive manufacture of all-oxide ferroelectric multilayer capacitors/transducers. Printed multilayer devices offer a significant increase in the capacitance density and the electromechanical voltage response in comparison to the single-layer devices. Further growth in the number of available functional oxide inks will enable arbitrary device architectures with novel functionalities.

Although carbon nanotube transistors present outstanding performances based on key metrics, large-scale uniformity and repeatability required in printable electronics depend greatly on proper control of the electrostatic environment. Through a survey of polymer dielectric encapsulants compatible with printing processes, a simple correlation is found between the measured interfacial charge density and the onset of conduction in a transistor, providing a rational route to control the electrical characteristics of carbon nanotube transistors. Smooth and continuous balancing of the properties between unipolar p-type and n-type transport is achieved using a molar fraction series of poly(styrene- co -2-vinylpyridine) statistical copolymers combined with an electron-donating molecule. We further demonstrate the easy fabrication of a p-n diode which shows a modest rectification of 8:1.

Microelectrode arrays (MEAs) are widely used platforms in bioelectronics to study electrogenic cells. In recent years, the processing of conductive polymers for the fabrication of three-dimensional electrode arrays has gained increasing interest for the development of novel sensor designs. Here, additive manufacturing techniques are promising tools for the production of MEAs with three-dimensional electrodes. In this work, a facile additive manufacturing process for the fabrication of MEAs that feature needle-like electrode tips, so-called μ-needles, is presented. To this end, an aerosol-jet compatible PEDOT:PSS and multiwalled carbon nanotube composite ink with a conductivity of 323 ± 75 S m -1 is developed and used in a combined inkjet and aerosol-jet printing process to produce the μ-needle electrode features. The μ-needles are fabricated with a diameter of 10 ± 2 μm and a height of 33 ± 4 μm. They penetrate an inkjet-printed dielectric layer to a height of 12 ± 3 μm. After successful printing, the electrochemical properties of the devices are assessed via cyclic voltammetry and impedance spectroscopy. The μ-needles show a capacitance of 242 ± 70 nF at a scan rate of 5 mV s -1 and an impedance of 128 ± 22 kΩ at 1 kHz frequency. The stability of the μ-needle MEAs in aqueous electrolyte is demonstrated and the devices are used to record extracellular signals from cardiomyocyte-like HL-1 cells. This proof-of-principle experiment shows the μ-needle MEAs' cell-culture compatibility and functional integrity to investigate electrophysiological signals from living cells.

Conductive inks for the future printed electronics should have the following merits: high conductivity, flexibility, low cost, and compatibility with wide range of substrates. However, the state-of-the-art conductive inks based on metal nanoparticles are high in cost and poor in flexibility. Herein, we reported a highly conductive, low cost, and super flexible ink based on graphene nanoplatelets. The graphene ink has been screen-printed on plastic and paper substrates. Combined with postprinting treatments including thermal annealing and compression rolling, the printed graphene pattern shows a high conductivity of 8.81 × 10 4 S m -1 and good flexibility without significant conductivity loss after 1000 bending cycles. We further demonstrate that the printed highly conductive graphene patterns can act as current collectors for supercapacitors. The supercapacitor with the printed graphene pattern as the current collector and printed activated carbon as the active material shows a good rate capability of up to 200 mV s -1 . This work potentially provides a promising route toward the large-scale fabrication of low cost yet flexible printed electronic devices.

Dynamic surfaces play a critical role in templating highly ordered complex structures in living systems but are rarely employed for directing assembly of synthetic functional materials. We design ion gel templates with widely tunable dynamics ( T g ) to template solution-coated conjugated polymers. We hypothesize that the ion gel expedites polymer nucleation by reconfiguring its surface to facilitate cooperative multivalent interactions with the conjugated polymer, validated using both experimental and computational approaches. Varying ion gel dynamics enables large modulation of alignment, molecular orientation, and crystallinity in templated polymer thin films. At the optimal conditions, ion-gel-templated films exhibit 55 times higher dichroic ratio (grazing incidence X-ray diffraction) and 49% increase in the relative degree of crystallinity compared to those templated by the neat polymer matrix. As a result, the maximum hole mobilities increase by factors of 4 and 11 along the π-π stacking and the backbone directions. Intriguingly, we observe a synergistic effect between the gel matrix and the ionic liquid that produces markedly enhanced templating effect than either component alone. Molecular dynamics simulations suggest that complementary multivalent interactions facilitated by template reconfigurability underlie the observed synergy. We further demonstrate field-effect transistors both templated and gated by ion gels with average mobility exceeding 7 cm 2 V -1 s -1 .

Photosensitive precursors are developed for the printing of 2D and 3D conductive structures via blue laser projection printing. With the assistance of a photosensitizer, metal nanoparticles can be efficiently photosynthesized under laser irradiation of low light intensity (45-290 mW cm -2 ). By projecting well-defined laser patterns on the precursor, corresponding 2D metal structures with the finest line of about 50 μm can be formed on various substrates including flexible polymer thin films, curved substrates, and ground glass. Moreover, complex 3D objects with nanoparticles embedded in the polymeric matrix are constructed via 3D printing combining photoreduction of the metal precursor and photopolymerization of resin. The as-prepared structures exhibit promising conductivities after sintering (in the order of magnitude of 10 6 S m -1 ). A possible mechanism of photochemical synthesis of metal nanoparticles upon exposure to blue laser is proposed. The high efficiency and low cost of the technique, the complexity of the structures prepared, and the applicability to various substrates and metals (including silver, gold, and palladium) promise practical applications of this approach in the printed electronics industry.

With the blooming of wearable technology, developing active materials that can be printed on a large scale has been attracting great attention. Particularly, there are abundant genius structure designs in nature that are endowed with superior performance, inspiring the design of materials for high-performance wearables. Herein, we report the controllable preparation of bionic carbon nanosheets decorated with in situ formed nanoparticles (NP-CNS) through the pyrolysis of calcium gluconate (CG), which are further used for printing high-performance humidity/pressure/strain sensors. The transformation from CG to NP-CNS had been studied in detail. Interestingly, papillae-like CaO NPs are formed on the carbon nanosheets, endowing NP-CNS with good dispersion in inks and rapid response to external stimuli. Particularly, the printed humidity sensor possesses a fast response time (1.7 s) and a broad detection range (0-96% RH), increasing from the high hydroscopicity of the CaO NPs and the thus induced expansion of the NP-CNS. Besides, the strain sensor and pressure sensor also show high sensitivity and broad detection range, which is derived from the unique bionic structure of the NP-CNS. We further showed their excellent performance in monitoring of pulse wave, breath, and human motion, indicating the wide potential applications of the bionic NP-CNS in smart wearables.