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 CO2 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.

Carbon nanomaterials such as graphene exhibit unique material properties such as high electrical conductivity, surface area, and biocompatibility that have the potential to significantly improve the performance of electrochemical sensors. Since in-field electrochemical sensors are typically disposable, they require materials that are amenable to low-cost, high-throughput, and scalable manufacturing. Conventional graphene devices based on low-yield chemical vapor deposition techniques are too expensive for such applications, while low-cost alternatives such as screen and inkjet printing do not possess sufficient control over electrode geometry to achieve favorable electrochemical sensor performance. In this work, aerosol jet printing (AJP) is used to create high-resolution (~40 µm line width) interdigitated electrodes (IDEs) on flexible substrates, which are then converted into histamine sensors by covalently linking monoclonal antibodies to oxygen moieties created on the graphene surface through a CO2 thermal annealing process. The resulting electrochemical sensors exhibit a wide histamine sensing range of 6. 25-200 ppm (56.25 µM -1.8 mM) and a low detection limit of 3.41 ppm (30.7 µM) within actual tuna broth samples. These sensor metrics are significant since histamine levels over 50 ppm in fish induce adverse health effects including severe allergic reactions (e.g., Scombroid food poisoning).Beyond the histamine case study presented here, the AJP and functionalization process can likely be generalized to a diverse range of sensing applications including environmental toxin detection, foodborne pathogen detection, wearable health monitoring, and health diagnostics.

Rapid, inexpensive, and easy-to-use coronavirus disease 2019 (COVID-19) home tests are key tools in addition to vaccines in the world-wide fight to eliminate national and local shutdowns. However, currently available tests for SARS-CoV-2, the virus that causes COVID-19, are too expensive, painful, and irritating, or not sufficiently sensitive for routine, accurate home testing. Herein, we employ custom-formulated graphene inks and aerosol jet printing (AJP) to create a rapid electrochemical immunosensor for direct detection of SARS-CoV-2 Spike Receptor-Binding Domain (RBD) in saliva samples acquired non-invasively. This sensor demonstrated limits of detection that are considerably lower than most commercial SARS-CoV-2 antigen tests (22.91 ± 4.72 pg/mL for Spike RBD and 110.38 ± 9.00 pg/mL for Spike S1) as well as fast response time (~30 mins), which was facilitated by the functionalization of printed graphene electrodes in a single-step with SARS-CoV-2 polyclonal antibody through the carbodiimide reaction without the need for nanoparticle functionalization or secondary antibody or metallic nanoparticle labels. This immunosensor presents a wide linear sensing range from 1 to 1000 ng/mL and does not react with other coexisting influenza viruses such as H1N1 hemagglutinin. By combining high-yield graphene ink synthesis, automated printing, high antigen selectivity, and rapid testing capability, this work offers a promising alternative to current SARS-CoV-2 antigen tests.

Printed 2D materials, derived from solution‐processed inks, offer scalable and cost‐effective routes to mechanically flexible optoelectronics. With micrometer‐scale control and broad processing latitude, aerosol‐jet printing (AJP) is of particular interest for all‐printed circuits and systems. Here, AJP is utilized to achieve ultrahigh‐responsivity photodetectors consisting of well‐aligned, percolating networks of semiconducting MoS2 nanosheets and graphene electrodes on flexible polyimide substrates. Ultrathin (≈1.2 nm thick) and high‐aspect‐ratio (≈1 μm lateral size) MoS2 nanosheets are obtained by electrochemical intercalation followed by megasonic atomization during AJP, which not only aerosolizes the inks but also further exfoliates the nanosheets. The incorporation of the high‐boiling‐point solvent terpineol into the MoS2 ink is critical for achieving a highly aligned and flat thin‐film morphology following AJP as confirmed by grazing‐incidence wide‐angle X‐ray scattering and atomic force microscopy. Following AJP, curing is achieved with photonic annealing, which yields quasi‐ohmic contacts and photoactive channels with responsivities exceeding 103 A W−1 that outperform previously reported all‐printed visible‐light photodetectors by over three orders of magnitude. Megasonic exfoliation coupled with properly designed AJP ink formulations enables the superlative optoelectronic properties of ultrathin MoS2 nanosheets to be preserved and exploited for the scalable additive manufacturing of mechanically flexible optoelectronics.

Memristive systems present a low-power alternative to silicon-based electronics for neuromorphic and in-memory computation. 2D materials have been increasingly explored for memristive applications due to their novel biomimetic functions, ultrathin geometry for ultimate scaling limits, and potential for fabricating large-area, flexible, and printed neuromorphic devices. While the switching mechanism in memristors based on single 2D nanosheets is similar to conventional oxide memristors, the switching mechanism in nanosheet composite films is complicated by the interplay of multiple physical processes and the inaccessibility of the active area in a twoterminal vertical geometry. Here, the authors report thermally activated memristors fabricated from percolating networks of diverse solution-processed 2D semiconductors including MoS 2 , ReS 2 , WS 2 , and InSe. The mechanisms underlying threshold switching and negative differential resistance are elucidated by designing large-area lateral memristors that allow the direct observation of filament and dendrite formation using in situ spatially resolved optical, chemical, and thermal analyses. The high switching ratios (up to 10 3 ) that are achieved at low fields (≈4 kV cm −1 ) are explained by thermally assisted electrical discharge that preferentially occurs at the sharp edges of 2D nanosheets. Overall, this work establishes percolating networks of solutionprocessed 2D semiconductors as a platform for neuromorphic architectures.

The demand for flexible biochemical sensors has increased with advances in computational functionality and wireless communication. Advances in materials science and biochemistry have enabled the development and fabrication of biosensors for selective detection of biological analytes leveraging ink-printed technologies, including in flexible form-factors. However, despite these advances, minimal effort has been devoted to translating the multi-material, three-electrode electrochemical cell, which is widely regarded as the standard for laboratory-scale studies, into a flexible form-factor for use in immunosensors, especially in a manner that is compatible with rapid and scalable additive manufacturing. Here, we report a fully printed and flexible electrochemical non-enzymatic immunosensor platform that integrates four chemically compatible inks and a non-covalent, two-step biofunctionalization scheme. The robustness of the platform is demonstrated using a model aptasensor that enables lysozyme detection using both electrochemical impedance spectroscopy and square wave voltammetry. The flexible, fully ink-printed aptasensor shows competitive performance to commercially available rod/disc electrodes in a bath cell. Overall, this work establishes a methodology for high-throughput fabrication of robust, flexible, multi-material, three-electrode immunosensors that can be generalized to a range of biosensor applications.

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Measuring the maximum operating temperature within the channel of ultrawide band-gap transistors is critically important since the temperature dependence of the device reliability sets operational limits such as maximum operational power. Thermoreflectance imaging (TTI) is an optimal choice to measure the junction temperature due to its submicrometer spatial resolution and submicrosecond temporal resolution. Since TTI is an imaging technique, data acquisition is orders of magnitude faster than point measurement techniques such as Raman thermometry. Unfortunately, commercially available LED light sources used in thermoreflectance systems are limited to energies less than ∼3.9 eV, which is below the band gap of many ultrawide band-gap semiconductors (>4.0 eV). Therefore, the semiconductors are transparent to the probing light sources, prohibiting the application of TTI. To address this thermal imaging challenge, we utilize an MoS 2 coating as a thermoreflectance enhancement coating that allows for the measurement of the surface temperature of (ultra)wide band-gap materials. The coating consists of a network of MoS 2 nanoflakes with the c axis aligned normal to the surface and is easily removable via sonication. The method is validated using electrical and thermal characterization of GaN and AlGaN devices. We demonstrate that this coating does not measurably influence the electrical performance or the measured operating temperature. A maximum temperature rise of 49 K at 0.59 W was measured within the channel of the AlGaN device, which is over double the maximum temperature rise obtained by measuring the thermoreflectance of the gate metal. The importance of accurately measuring the peak operational temperature is discussed in the context of accelerated stress testing.