Mobile Efficient Diagnostics of Infectious Diseases via On-Chip RT-qPCR: MEDIC-PCR.

The COVID-19 outbreak has caused public and global health crises. However, the lack of on-site fast, reliable, sensitive, and low-cost reverse transcription polymerase chain reaction (RT-PCR) testing limits early detection, timely isolation, and epidemic prevention and control. Here, the authors report a rapid mobile efficient diagnostics of infectious diseases via on-chip -RT-quantitative PCR (RT-qPCR): MEDIC-PCR. First, the authors use a roll-to-roll printing process to accomplish low-cost carbon-black-based disposable PCR chips that enable rapid LED-induced photothermal PCR cycles. The MEDIC-PCR can perform RT (3 min), and PCR (9 min) steps. Further, the cohort of 89 COVID-19 and 103 non-COVID-19 patients testing is completed by the MEDIC-PCR to show excellent diagnostic accuracy of 97%, sensitivity of 94%, and specificity of 98%. This MEDIC-PCR can contribute to the preventive global health in the face of a future pandemic.

Tuning the charge carrier polarity of roll-to-roll gravure printed carbon nanotube-based thin film transistors by an atomic layer deposited alumina nanolayer.

Charge carrier polarity tuning in printed thin film transistors (TFTs) is a crucial step in order to obtain complementary printed devices. In this work, we studied the effect of an Al2O3 passivation layer on printed single-walled carbon nanotube (SWCNT) based TFTs to tune the charge carrier polarity. By varying the atomic layer deposition (ALD) temperature and Al2O3 layer thickness, we can tune the doping degree of Al2O3 to tailor the polarity of printed SWCNT-based TFTs (SWCNT-TFTs). The precise control of threshold voltage (Vth) and polarity from p-type to well-balanced ambipolar, and n-type SWCNT-TFTs is successfully demonstrated with high repeatability by optimizing the ALD temperature and Al2O3 layer thickness based on 20 printed samples per test. As a proof-of-concept, inverter logic circuits using the SWCNT-TFT with different polarity types are demonstrated. The ambipolar device-based inverter exhibits a voltage gain of 3.9 and the CMOS-based inverter exhibits a gain of approximately 4.3, which is comparable to the current roll-to-roll (R2R) printed inverter circuits. Different thicknesses of Al2O3 layer, coated by the ALD at different temperatures and thicknesses, provide a deep understanding of the device fabrication and control process to implement the tailored doping method to efficiently realize R2R printed SWCNT-TFT-based complementary electronic devices.

Towards Digital Twin Implementation in Roll-To-Roll Gravure Printed Electronics: Overlay Printing Registration Error Prediction Based on Printing Process Parameters.

Roll-to-roll gravure (R2Rg) has become highly affiliated with printed electronics in the past few years due to its high yield of printed thin-film transistor (TFT) in active matrix devices, and to its low cost. For printing TFTs with multilayer structures, achieving a high-precision in overlay printing registration accuracy (OPRA) is a key challenge to attain the high degree of TFT integration through R2Rg. To address this challenge efficiently, a digital twin paradigm was first introduced in the R2Rg system with an aim to optimize the OPRA by developing a predictive model based on typical input variables such as web tension, nip force, and printing speed in the R2Rg system. In our introductory-level digital twin, errors in the OPRA were collected with the variable parameters of web tensions, nip forces, and printing speeds from several R2Rg printing processes. Subsequently, statistical features were extracted from the input data followed by the training of a deep learning long-short term memory (LSTM) model for predicting machine directional error (MD) in the OPRA. As a result of training the LSTM model in our digital twin, its attained accuracy of prediction was 77%. Based on this result, we studied the relationship between the nip forces and printing speeds to predict the MD error in the OPRA. The results indicated a correlation between the MD error in the OPRA and the printing speed, as the MD error amplitude in the OPRA tended to decline at the higher printing speed.

Improving Stability of Roll-to-Roll (R2R) Gravure-Printed Carbon Nanotube-Based Thin Film Transistors via R2R Plasma-Enhanced Chemical Vapor-Deposited Silicon Nitride.

Single-walled carbon nanotubes (SWCNTs) have an advantage in printing thin film transistors (TFTs) due to their high carrier mobility, excellent chemical stability, mechanical flexibility, and compatibility with solution-based processing. Thus, the printed SWCNT-based TFTs (pSWCNT-TFTs) showed significant technological potential such as integrated circuits, conformable sensors, and display backplanes. However, the long-term environmental stability of the pSWCNT-TFTs hinders their commercialization. Thus, to extend the stability of the pSWCNT-TFTs, such devices should be passivated with low water and oxygen permeability. Herein, we introduced the silicon nitride (SiNx) passivation method on the pSWCNT-TFTs via a combination of roll-to-roll (R2R) gravure and the roll-to-roll plasma-enhanced vapor deposition (R2R-PECVD) process at low temperature (45 °C). We found that SiNx-passivated pSWCNT-TFTs showed ± 0.50 V of threshold voltage change at room temperature for 3 days and ±1.2 V of threshold voltage change for 3 h through a Temperature Humidity Test (85/85 test: Humidity 85%/Temperature 85 °C) for both p-type and n-type pSWCNT-TFTs. In addition, we found that the SiNx-passivated p-type and n-type pSWCNT-TFT-based CMOS-like ring oscillator, or 1-bit code generator, operated well after the 85/85 test for 24 h.

Rapid Uniformity Analysis of Fully Printed SWCNT-Based Thin Film Transistor Arrays via Roll-to-Roll Gravure Process.

The roll-to-roll (R2R) gravure process has the potential for manufacturing single-wall carbon nanotubes (SWCNT)-based thin film transistor (TFT) arrays on a flexible plastic substrate. A significant hurdle toward the commercialization of the R2R-printed SWCNT-TFT array is the lack of a suitable, simple, and rapid method for measuring the uniformity of printed products. We developed a probing instrument for characterizing R2R gravure printed TFT, named PICR2R-TFT, for rapidly characterizing R2R-printed SWCNT-TFT array that can present a geographical distribution profile to pinpoint the failed devices in an SWCNT-TFT array. Using the newly developed PICR2R-TFT instrument, the current-voltage characteristics of the fabricated SWCNT-TFT devices could be correlated to various R2R-printing process parameters, such as channel length, roll printing length, and printing speed. Thus, by introducing a characterization tool that is reliable and fast, one can quickly optimize the R2R gravure printing conditions to enhance product uniformity, thereby maximizing the yield of printed SWCNT-TFT arrays.

Proving the robustness of a PEDOT:PSS-based thermistor via functionalized graphene oxide-poly(vinylidene fluoride) composite encapsulation for food logistics.

The instability of poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) under a humid condition is the major limitation in the practical development of a flexible thermistor. Here, we introduced a functionalized graphene oxide-polyvinylidene fluoride (FGO-PVDF) composite as an encapsulation layer to prove the reliability of PEDOT:PSS thermistors under high-humidity conditions. The FGO-PVDF-encapsulated thermistor exhibited good linearity, a resolution of 1272.57 Ω per °C, a temperature coefficient of resistance equal to -3.95 × 10-3 per °C, stable performance, and an acceptable response time (∼40 s per °C) calibrated in the temperature range between -10 °C and 30 °C, resembling the temperature of a cold chain system. For applications in a food cold chain system, this thermistor was integrated into a roll-to-roll (R2R) gravure-printed NFC antenna, a microcontroller-embedded Si-chip transponder, and a printed battery to work as a smart label to wirelessly monitor the time-temperature history (TTH) of a food package. A proof-of-concept study was demonstrated by attaching an NFC-enabled hybrid TTH logger, a smart label, in a chicken package.

Roll-to-Roll Gravure Printed Electrochemical Sensors for Wearable and Medical Devices.

As recent developments in noninvasive biosensors spearhead the thrust toward personalized health and fitness monitoring, there is a need for high throughput, cost-effective fabrication of flexible sensing components. Toward this goal, we present roll-to-roll (R2R) gravure printed electrodes that are robust under a range of electrochemical sensing applications. We use inks and electrode morphologies designed for electrochemical and mechanical stability, achieving devices with uniform redox kinetics printed on 150 m flexible substrate rolls. We show that these electrodes can be functionalized into consistently high performing sensors for detecting ions, metabolites, heavy metals, and other small molecules in noninvasively accessed biofluids, including sensors for real-time, in situ perspiration monitoring during exercise. This development of robust and versatile R2R gravure printed electrodes represents a key translational step in enabling large-scale, low-cost fabrication of disposable wearable sensors for personalized health monitoring applications.

Methylxanthine Drug Monitoring with Wearable Sweat Sensors.

Drug monitoring plays crucial roles in doping control and precision medicine. It helps physicians tailor drug dosage for optimal benefits, track patients' compliance to prescriptions, and understand the complex pharmacokinetics of drugs. Conventional drug tests rely on invasive blood draws. While urine and sweat are attractive alternative biofluids, the state-of-the-art methods require separate sample collection and processing steps and fail to provide real-time information. Here, a wearable platform equipped with an electrochemical differential pulse voltammetry sensing module for drug monitoring is presented. A methylxanthine drug, caffeine, is selected to demonstrate the platform's functionalities. Sweat caffeine levels are monitored under various conditions, such as drug doses and measurement time after drug intake. Elevated sweat caffeine levels upon increasing dosage and confirmable caffeine physiological trends are observed. This work leverages a wearable sweat sensing platform toward noninvasive and continuous point-of-care drug monitoring and management.

Proving Scalability of an Organic Semiconductor To Print a TFT-Active Matrix Using a Roll-to-Roll Gravure.

Organic semiconductor-based thin-film transistors' (TFTs) charge-carrier mobility has been enhanced up to 25 cm2/V s through the improvement of fabrication methods and greater understanding of the microstructure charge-transport mechanism. To expand the practical feasibility of organic semiconductor-based TFTs, their electrical properties should be easily accessed from the fully printed devices through a scalable printing method, such as a roll-to-roll (R2R) gravure. In this study, four commercially available organic semiconductors were separately formulated into gravure inks. They were then employed in the R2R gravure system (silver ink for printing gate and drain-source electrodes and BaTiO3 ink for printing dielectric layers) for printing 20 × 20 TFT-active matrix with the resolution of 10 pixels per inch on poly(ethylene terephthalate) (PET) foils to attain electrical properties of organic semiconductors a practical printing method. Electrical characteristics (mobility, on-off current ratio, threshold voltage, and transconductance) of the R2R gravure-printed 20 × 20 TFT-active matrices fabricated with organic semiconducting ink were analyzed statistically, and the results showed more than 98% device yield and 50 % electrical variations in the R2R gravure TFT-active matrices along the PET web.

Fully gravure printed complementary carbon nanotube TFTs for a clock signal generator using an epoxy-imine based cross-linker as an n-dopant and encapsulant.

Printed p-type single walled carbon nanotube (SWCNT) based circuits exhibit high power dissipation owing to their thick printed dielectric layers (>2 µm) and long channels (>100 µm). In order to reduce the static power dissipation of printed SWCNT-base circuits while maintaining the same printing conditions and channel lengths, complementary metal-oxide-semiconductor (CMOS) based circuits are more ideal. These circuits, however, have not been successfully implemented in a scalable printing platform due to unstable threshold voltages of n-doped SWCNT based thin film transistors (TFTs). In this work, a thermally curable epoxy-imine-based n-doping ink is presented for achieving uniform doping and sealing of SWCNT layers by gravure printing. After printing the n-doping ink, the ink is cured to initiate a cross-linking reaction to seal the n-doped SWCNT-TFTs so that the threshold voltage of the n-doped SWCNT-TFTs is stabilized. Flexible CMOS ring oscillators using such n-doped SWCNT-TFTs combined with the intrinsically p-type SWCNT-TFTs can generate a 0.2 Hz clock signal with significantly lower power consumption compared to similarly printed p-type only TFT based ring oscillators. Moving forward, this CMOS flexible ring oscillator can be practically used to develop fully printed inexpensive wireless sensor tags.

Fully Printed and Encapsulated SWCNT-Based Thin Film Transistors via a Combination of R2R Gravure and Inkjet Printing.

Fully printed thin film transistors (TFT) based on poly(9,9-di-n-dodecylfluorene) (PFDD) wrapped semiconducting single walled carbon nanotube (SWCNT) channels are fabricated by a practical route that combines roll-to-roll (R2R) gravure and ink jet printing. SWCNT network density is easily controlled via ink formulation (concentration and polymer:CNT ratio) and jetting conditions (droplet size, drop spacing, and number of printed layers). Optimum inkjet printing conditions are established on Si/SiO2 in which an ink consisting of 6:1 PFDD:SWCNT ratio with 50 mg L-1 SWCNT concentration printed at a drop spacing of 20 µm results in TFTs with mobilities of ∼25 cm2 V-1 s-1 and on-/off-current ratios > 105. These conditions yield excellent network uniformity and are used in a fully additive process to fabricate fully printed TFTs on PET substrates with mobility values > 5 cm2 V-1 s-1 (R2R printed gate electrode and dielectric; inkjet printed channel and source/drain electrodes). An inkjet printed encapsulation layer completes the TFT process (fabricated in bottom gate, top contact TFT configuration) and provides mobilities > 1 cm2 V-1 s-1 with good operational stability, based on the performance of an inverter circuit. An array of 20 TFTs shows that most have less than 10% variability in terms of threshold voltage, transconductance, on-current, and subthreshold swing.

Fully printed flexible and disposable wireless cyclic voltammetry tag.

A disposable cyclic voltammetry (CV) tag is printed on a plastic film by integrating wireless power transmitter, polarized triangle wave generator, electrochemical cell and signage through a scalable gravure printing method. By proximity of 13.56 MHz RF reader, the printed CV tag generates 320 mHz of triangular sweep wave from +500 mV to -500 mV which enable to scan a printed electrochemical cell in the CV tag. By simply dropping any specimen solution on the electrochemical cell in the CV tag, the presence of solutes in the solution can be detected and shown on the signage of the CV tag in five sec. 10 mM of N,N,N',N'-tetramethyl-p-phenylenediamine (TMPD) was used as a standard solute to prove the working concept of fully printed disposable wireless CV tag. Within five seconds, we can wirelessly diagnose the presence of TMPD in the solution using the CV tag in the proximity of the 13.56 MHz RF reader. This fully printed and wirelessly operated flexible CV tag is the first of its kind and marks the path for the utilization of inexpensive and disposable wireless electrochemical sensor systems for initial diagnose hazardous chemicals and biological molecules to improve public hygiene and health.