Flexible, Print-in-Place 1D-2D Thin-Film Transistors Using Aerosol Jet Printing

In this work, we overcome temperature constraints and demonstrate 1D−2D thin-film transistors (1D−2D TFTs) in a low-temperature (maximum exposure ≤80 °C) full print-in-place process (i.e., no substrate removal from printer throughout the entire process) using an aerosol jet printer. Semiconducting 1D CNT channels are used with a 2D hexagonal boron nitride (h-BN) gate dielectric and traces of silver nanowires as the conductive electrodes, all deposited using the same printer. The aerosol jet-printed 2D h-BN films were realized via proper ink formulation, such as utilizing the binder hydroxypropyl methylcellulose, which suppresses redispersion between adjacent printed layers. In addition to an ON/ OFF current ratio up to 3.5 Å~ 105, channel mobility up to 10.7 cm2·V-1·s-1, and low gate hysteresis, 1D−2D TFTs exhibit extraordinary mechanical stability under bending due to the nanoscale network structure of each layer, with minimal changes in performance after 1000 bending test cycles at 2.1% strain. It is also confirmed that none of the device layers require high-temperature treatment to realize optimal performance. These findings provide an attractive approach toward a cost-effective, direct-write realization of electronics

Additive Manufacturing of Electrically Conductive Multi-Layered Nanocopper in an Air Environment

The additive manufacturing (AM) of functional copper (Cu) parts is a major goal for many industries, from aerospace to automotive to electronics, because Cu has a high thermal and electrical conductivity as well as being ~10× cheaper than silver. Previous studies on AM of Cu have concentrated mainly on high-energy manufacturing processes such as Laser Powder Bed Fusion, Electron Beam Melting, and Binder Jetting. These processes all require high-temperature heat treatment in an oxygen-free environment. This paper shows an AM route to multi-layered microparts from novel nanoparticle (NP) Cu feedstocks, performed in an air environment, employing a low-power (<10 W) laser sintering process. Cu NP ink was deposited using two mechanisms, inkjet printing, and bar coating, followed by low-power laser exposure to induce particle consolidation. Initial parts were manufactured to a height of approximately 100 µm, which was achieved by multi-layer printing of 15 (bar-coated) to 300 (inkjetted) layers. There was no evidence of oxidised copper in the sintered material, but they were found to be low-density, porous structures. Nonetheless, electrical resistivity of ~28 × 10−8 Ω m was achieved. Overall, the aim of this study is to offer foundational knowledge for upscaling the process to additively manufacture Cu 3D parts of significant size via sequential nanometal ink deposition and low-power laser processing

Raman Fingerprints of Graphene Produced by Anodic Electrochemical Exfoliation

Electrochemical exfoliation is one of the most promising methods for scalable production of graphene. However, limited understanding of its Raman spectrum as well as lack of measurement standards for graphene strongly limit its industrial applications. In this work we show a systematic study of the Raman spectrum of electrochemically exfoliated graphene, produced using different electrolytes and different types of solvents in varying amounts. We demonstrate that no information on the thickness can be extracted from the shape of the 2D peak as this type of graphene is defective. Furthermore, the number of defects and the uniformity of the samples strongly depend on the experimental conditions, including post-processing. Under specific conditions, formation of short conductive trans-polyacetylene chains has been observed. Our Raman analysis provides guidance for the community on how to get information on defects coming from electrolyte, temperature and other experimental conditions, by making Raman spectroscopy a powerful metrology tool.Comment: This document is the unedited Author's version of a Submitted Work that was subsequently accepted for publication in Nano Letters, American Chemical Society after peer review. To access the final edited and published work, included the SI, see DOI: 10.1021/acs.nanolett.0c0033

Inkjet-printed graphene Hall mobility measurements and low-frequency noise characterization

We report room-temperature Hall mobility measurements, low-temperature magnetoresistance analysis, and low-frequency noise characterization of inkjet-printed graphene films on fused quartz and SiO2/Si substrates. We found that thermal annealing in vacuum at 450 ◦C is a necessary step in order to stabilize the Hall voltage across the devices, allowing their electrical characterization. The printed films present a minimum sheet resistance of 23.3 Ω/sq after annealing, and are n-type doped, with carrier concentrations in the low 1020 cm−3 range. The charge carrier mobility is found to increase with increasing film thickness, reaching a maximum value of 33 cm2 V−1 s−1 for a 480 nm-thick film printed on SiO2/Si. Low-frequency noise characterization shows a 1/f noise behavior and a Hooge parameter in the range of 0.1 – 1. These results represent the first in-depth electrical and noise characterization of transport in inkjet-printed graphene films, able to provide physical insights on the mechanisms at play

Formulation of functional materials for inkjet printing: A pathway towards fully 3D printed electronics

Inkjet printing offers a facile route for manufacturing the next generation of electronic devices, by combining the design freedom of additive manufacturing technologies with tuneable properties of functional materials and opportunities for their integration into heterostructures. However, to fully realise this potential, the library of functional materials available for additive manufacturing technologies needs to be expanded. In this review, we summarise current developments in ink formulation strategies, approaches for tailoring the functional properties of inks, and multi-material processing. Material – process – property relationships are reviewed for emerging functional materials, such as polymers, nanomaterials, and composites, with examples of current state-of-the-art devices. The flexibility of combining inkjet deposition with other existing technologies and a variety of substrates is also discussed reviewing current trends in electronics and optoelectronics, including wearable electronics, sensing, and energy applications. The review offers a comprehensive and systematic overview of ink formulations for inkjet deposition of electronic devices, summarising the challenges and perspectives in the advancement of 3D and multi-functional electronic devices and smart electronics

Multiorgan MRI findings after hospitalisation with COVID-19 in the UK (C-MORE): a prospective, multicentre, observational cohort study

Introduction: The multiorgan impact of moderate to severe coronavirus infections in the post-acute phase is still poorly understood. We aimed to evaluate the excess burden of multiorgan abnormalities after hospitalisation with COVID-19, evaluate their determinants, and explore associations with patient-related outcome measures. Methods: In a prospective, UK-wide, multicentre MRI follow-up study (C-MORE), adults (aged ≥18 years) discharged from hospital following COVID-19 who were included in Tier 2 of the Post-hospitalisation COVID-19 study (PHOSP-COVID) and contemporary controls with no evidence of previous COVID-19 (SARS-CoV-2 nucleocapsid antibody negative) underwent multiorgan MRI (lungs, heart, brain, liver, and kidneys) with quantitative and qualitative assessment of images and clinical adjudication when relevant. Individuals with end-stage renal failure or contraindications to MRI were excluded. Participants also underwent detailed recording of symptoms, and physiological and biochemical tests. The primary outcome was the excess burden of multiorgan abnormalities (two or more organs) relative to controls, with further adjustments for potential confounders. The C-MORE study is ongoing and is registered with ClinicalTrials.gov, NCT04510025. Findings: Of 2710 participants in Tier 2 of PHOSP-COVID, 531 were recruited across 13 UK-wide C-MORE sites. After exclusions, 259 C-MORE patients (mean age 57 years [SD 12]; 158 [61%] male and 101 [39%] female) who were discharged from hospital with PCR-confirmed or clinically diagnosed COVID-19 between March 1, 2020, and Nov 1, 2021, and 52 non-COVID-19 controls from the community (mean age 49 years [SD 14]; 30 [58%] male and 22 [42%] female) were included in the analysis. Patients were assessed at a median of 5·0 months (IQR 4·2–6·3) after hospital discharge. Compared with non-COVID-19 controls, patients were older, living with more obesity, and had more comorbidities. Multiorgan abnormalities on MRI were more frequent in patients than in controls (157 [61%] of 259 vs 14 [27%] of 52; p&lt;0·0001) and independently associated with COVID-19 status (odds ratio [OR] 2·9 [95% CI 1·5–5·8]; padjusted=0·0023) after adjusting for relevant confounders. Compared with controls, patients were more likely to have MRI evidence of lung abnormalities (p=0·0001; parenchymal abnormalities), brain abnormalities (p&lt;0·0001; more white matter hyperintensities and regional brain volume reduction), and kidney abnormalities (p=0·014; lower medullary T1 and loss of corticomedullary differentiation), whereas cardiac and liver MRI abnormalities were similar between patients and controls. Patients with multiorgan abnormalities were older (difference in mean age 7 years [95% CI 4–10]; mean age of 59·8 years [SD 11·7] with multiorgan abnormalities vs mean age of 52·8 years [11·9] without multiorgan abnormalities; p&lt;0·0001), more likely to have three or more comorbidities (OR 2·47 [1·32–4·82]; padjusted=0·0059), and more likely to have a more severe acute infection (acute CRP &gt;5mg/L, OR 3·55 [1·23–11·88]; padjusted=0·025) than those without multiorgan abnormalities. Presence of lung MRI abnormalities was associated with a two-fold higher risk of chest tightness, and multiorgan MRI abnormalities were associated with severe and very severe persistent physical and mental health impairment (PHOSP-COVID symptom clusters) after hospitalisation. Interpretation: After hospitalisation for COVID-19, people are at risk of multiorgan abnormalities in the medium term. Our findings emphasise the need for proactive multidisciplinary care pathways, with the potential for imaging to guide surveillance frequency and therapeutic stratification

Water-based and Inkjet Printable Inks made by Electrochemically Exfoliated Graphene

Inkjet printable graphene inks are very attractive for applications in flexible and foldable electronics, such as wearable electronics and the Internet of Things. However, the ink preparation is still very time consuming as high concentrations can be achieved only with prolonged sonication (>24 hours) or with expensive setups. Here we demonstrate a water-based inkjet printable ink made from electrochemically exfoliated graphene. A printable and stable (> 1 month) ink with concentration of ~2.25 mg mL-1 was formulated in less than 5 hrs, using two successive steps: first exfoliation and dispersion of large graphene flakes (> 5 um) followed by 1 hour tip-sonication to reduce the flake size below 1 um, as required for the material to be ejected by the nozzle. The formulated ink contains more than 75% single- and few-layers (i.e. less than 2 nm in thickness) graphene flakes with an average lateral size of 740 nm. Thermal annealing allows to achieve high C/O ratio (>10), which translates into one of the highest electrical conductivity (~3.91 x 104 S m-1) reported so far for solution-processed graphene, without the use of any harsh chemical processing.Comment: This article is accepted in Carbon and is available online (https://doi.org/10.1016/j.carbon.2019.04.047

All-Inkjet-Printed Graphene-Gated Organic Electrochemical Transistors on Polymeric Foil as Highly Sensitive Enzymatic Biosensors

We demonstrate fully inkjet-printed graphene-gated organic electrochemical transistors (OECTs) on polymeric foil for the enzymatic-based biosensing of glucose. The graphene-gated transistors exhibit better linearity, repeatability, and sensitivity than the printed silver-gated devices studied in this work and other types of printed devices previously reported in the literature. Their limit of detection is 100 nM with a normalized sensitivity of 20%/dec in the linear range of 30–5000 μM glucose concentrations, hence comparable with state-of-the-art OECT devices made by lithography processes on rigid substrates and with complex multilayer gates. Electrochemical impedance spectroscopy analysis shows that the improved sensitivity of the graphene-gated devices is related to a significant decrease of the charge-transfer resistance at the graphene electrode–electrolyte interface in the presence of glucose. The optimized sensing method and device configuration are also extended to the detection of the metabolite lactate. This study enables the development of fully printed high-performance enzymatic OECTs with graphene-sensing gates for multimetabolite sensing