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The continued proliferation of superbugs in hospitals and the coronavirus disease 2019 (COVID-19) has created an acute worldwide demand for sustained broadband pathogen suppression in households, hospitals, and public spaces. In response, we have created a highly active, self-sterilizing copper configuration capable of inactivating a wide range of bacteria and viruses in 30-60 seconds. The highly active material destroys pathogens faster than any conventional copper configuration and acts as quickly as alcohol wipes and hand sanitizers. Unlike the latter, our copper material does not release volatile compounds or leave harmful chemical residues and maintains its antimicrobial efficacy over sustained use; it is shelf stable for years. We have performed rigorous testing in accordance with guidelines from U.S. regulatory agencies and believe that the material could offer broad spectrum, non-selective defense against most microbes via integration into masks, protective equipment, and various forms of surface coatings.
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Anti-Infecciosos , COVID-19 , Antibacterianos , Humanos , Equipamento de Proteção Individual , SARS-CoV-2RESUMO
Solution coating of organic semiconductors offers great potential for achieving low-cost manufacturing of large-area and flexible electronics. However, the rapid coating speed needed for industrial-scale production poses challenges to the control of thin-film morphology. Here, we report an approach--termed fluid-enhanced crystal engineering (FLUENCE)--that allows for a high degree of morphological control of solution-printed thin films. We designed a micropillar-patterned printing blade to induce recirculation in the ink for enhancing crystal growth, and engineered the curvature of the ink meniscus to control crystal nucleation. Using FLUENCE, we demonstrate the fast coating and patterning of millimetre-wide, centimetre-long, highly aligned single-crystalline organic semiconductor thin films. In particular, we fabricated thin films of 6,13-bis(triisopropylsilylethynyl) pentacene having non-equilibrium single-crystalline domains and an unprecedented average and maximum mobilities of 8.1±1.2 cm(2) V(-1) s(-1) and 11 cm(2) V(-1) s(-1). FLUENCE of organic semiconductors with non-equilibrium single-crystalline domains may find use in the fabrication of high-performance, large-area printed electronics.
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MoO(x) has been used for organic semiconductor doping, but it had been considered an inefficient and/or unstable dopant. We report that MoO(x) can strongly and stably dope carbon nanotubes and graphene. Thermally annealed MoO(x)-CNT composites can form durable thin film electrodes with sheet resistances of 100 Ω/sq at 85% transmittance plain and 85 Ω/sq at 83% transmittance with a PEDOT:PSS adlayer. Sheet resistances change less than 10% over 20 days in ambient and less than 2% with overnight heating to 300 °C in air. The MoO(x) can be easily deposited either by thermal evaporation or from solution-based precursors. Excellent stability coupled with high conductivity makes MoO(x)-CNT composites extremely attractive candidates for practical transparent electrodes.
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The use of organic transistors as sensing platforms provides a number of distinct advantages over conventional detection technologies, including their tunability, portability, and ability to directly transduce binding events without tedious and expensive labeling procedures. However, detection efforts using organic transistors lack a general method to uniquely specify and detect a target of interest. While highly sensitive liquid- and vapor-phase sensors have been previously reported, detection has been restricted either to the serendipitous interaction of the analyte molecules with the organic semiconductor or to the covalent functionalization of the semiconductor with receptor groups to enhance specificity. However, the former technique cannot be regularly relied upon for tailorable sensing while the latter may result in unpredictable decreases in electronic performance. Thus, a method to provide modular receptor sites on the surface of an organic transistor without damaging the device will significantly advance the field, especially regarding biological species detection. In this work, we utilized a block copolymer to template ordered, large-area arrays of gold nanoparticles, with sub-100 nm center-to-center spacing onto the surface of an organic transistor. This highly modular platform is designed for orthogonal modification with a number of available chemical and biological functional groups by taking advantage of the well-studied gold-thiol linkage. Herein, we demonstrate the functionalization of gold nanoparticles with a mercury-binding oligonucleotide sequence. Finally, we demonstrate the highly selective and robust detection of mercury(II) using this platform in an underwater environment.
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Técnicas Biossensoriais/métodos , Ouro/química , Nanopartículas Metálicas/química , Nanotecnologia/instrumentação , Compostos Orgânicos/química , Transistores Eletrônicos , Alcenos/química , DNA/química , Poluentes Ambientais/análise , Poluentes Ambientais/química , Mercúrio/análise , Mercúrio/química , Polivinil/químicaRESUMO
Developing orthogonal surface chemistry techniques that perform at the nanoscale is key to achieving precise control over molecular patterning on surfaces. We report the formation and selective functionalization of alumina nanoparticle arrays generated from block copolymer templates. This new material provides an alternative to gold for orthogonal surface chemistry at the nanometer scale. Atomic force microscopy and X-ray photoelectron spectroscopy confirm these particles show excellent selectivity over silica for phosphonic and carboxylic acid adsorption. As this is the first reported synthesis of alumina nanoparticles from block copolymer templates, characterizations via Fourier transform infrared spectroscopy, Auger electron spectroscopy, and transmission electron microscopy are presented. Reproducible formation of alumina nanoparticles was dependent on a counterintuitive synthetic step wherein a small amount of water is added to an anhydrous toluene solution of block copolymer and aluminum chloride. The oxidation environment of the aluminum in these particles, as measured by Auger electron spectroscopy, is similar to that of native aluminum oxide and alumina grown by atomic layer deposition. This discovery expands the library of available surface chemistries for nanoscale molecular patterning.
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Óxido de Alumínio/química , Nanopartículas/química , Polímeros/química , Microscopia Eletrônica de Transmissão , Espectroscopia de Infravermelho com Transformada de Fourier , Propriedades de SuperfícieRESUMO
This study evaluates an alternative to electron-beam lithography for fabricating nanoscale graphene devices. Dip-pen nanolithography is used for defining monolayer graphene flakes and for patterning of gold electrodes through writing of an alkylthiol on thin films of gold evaporated onto graphene flakes. A wet gold etching step was used to form the individual devices. The sheet resistances of these monolayer graphene devices are comparable to reported literature values. This alternative technique for making electrical contact to 2D nanostructures provides a platform for fundamental studies of nanomaterial properties. The merits of using dip-pen nanolithography include lack of electron-beam irradiation damage and targeted patterning of individual devices with imaging and writing conducted in the same instrument under ambient conditions.
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Reduced graphene oxide (RGO) is an electrically conductive carbon-based nanomaterial that has recently attracted attention as a potential electrode for organic electronics. Here we evaluate several solution-based methods for fabricating RGO bottom-contact (BC) electrodes for organic thin-film transistors (OTFTs), demonstrate functional p- and n-channel devices with such electrodes, and compare their electrical performance with analogous devices containing gold electrodes. We show that the morphology of organic semiconductor films deposited on RGO electrodes is similar to that observed in the channel region of the devices and that devices fabricated with RGO electrodes have lower contact resistances compared to those fabricated with gold contacts. Although the conductivity of RGO is poor compared to that of gold, RGO is still an enticing electrode material for organic electronic devices possibly owing to the retention of desirable morphological features, lower contact resistance, lower cost, and solution processability.
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The development of an electronic skin is critical to the realization of artificial intelligence that comes into direct contact with humans, and to biomedical applications such as prosthetic skin. To mimic the tactile sensing properties of natural skin, large arrays of pixel pressure sensors on a flexible and stretchable substrate are required. We demonstrate flexible, capacitive pressure sensors with unprecedented sensitivity and very short response times that can be inexpensively fabricated over large areas by microstructuring of thin films of the biocompatible elastomer polydimethylsiloxane. The pressure sensitivity of the microstructured films far surpassed that exhibited by unstructured elastomeric films of similar thickness, and is tunable by using different microstructures. The microstructured films were integrated into organic field-effect transistors as the dielectric layer, forming a new type of active sensor device with similarly excellent sensitivity and response times.
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We report patterned deposition of carbon nanotube/conjugated polymer composites from solution with high nanotube densities and excellent feature resolution. Such composites are suited for use as electrodes in high-performance transistors of pentacene and C(60), with bottom-contact mobilities of > 0.5 and > 1 cm(2) V(−1) s(−1), respectively. This represents a clear step towards development of inexpensive, high-performance all-organic circuits.
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Nanotubos de Carbono/química , Compostos Organosselênicos/química , Soluções/química , Transistores Eletrônicos , Eletrodos , Fulerenos/química , Naftacenos/químicaRESUMO
The development of solution-processable, high-performance n-channel organic semiconductors is crucial to realizing low-cost, all-organic complementary circuits. Single-crystalline organic semiconductor nano/microwires (NWs/MWs) have great potential as active materials in solution-formed high-performance transistors. However, the technology to integrate these elements into functional networks with controlled alignment and density lags far behind their inorganic counterparts. Here, we report a solution-processing approach to achieve high-performance air-stable n-channel organic transistors (the field-effect mobility (mu) up to 0.24 cm(2)/Vs for MW networks) comprising high mobility, solution-synthesized single-crystalline organic semiconducting MWs (mu as high as 1.4 cm(2)/Vs for individual MWs) and a filtration-and-transfer (FAT) alignment method. The FAT method enables facile control over both alignment and density of MWs. Our approach presents a route toward solution-processed, high-performance organic transistors and could be used for directed assembly of various functional organic and inorganic NWs/MWs.
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Precise electrical contact between single-molecule and electrodes is a first step to study single-molecule electronics and its application such as (bio)sensors and nanodevices. To realize a reliable electrical contact, we can use DNA as a template in the field of nanoelectronics because of its micrometer-scaled length with the thickness of nanometer-scale. In this paper, we studied the reactivity of the amide-coupling reaction to tether oligodeoxynucleotides (ODNs) to organic molecules and the elongation of the ODNs by the polymerase chain reaction (PCR) to synthesize 1.5 kbp dsDNA-organic molecule-1.5 kbp dsDNA (DOD) triblock architecture. The successful amide-coupling reactions were confirmed by electrospray ionization mass spectrometry (ESI-MS), and the triblock architectures were characterized by 1% agarose gel electrophoresis and atomic force microscope (AFM). Our result shows that this strategy is simple and makes it easy to construct DNA-organic molecule-DNA triblock architectures and potentially provides a platform to prepare and investigate single molecule electronics.
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Amidas/química , DNA/química , Oligonucleotídeos/química , Reação em Cadeia da Polimerase/métodos , Bacteriófago lambda/química , Bacteriófago lambda/genética , DNA/síntese química , DNA Viral/química , Microeletrodos , Nanoestruturas/química , Oligonucleotídeos/síntese químicaRESUMO
We present a high performance, ambipolar organic field-effect transistor composed of a single material. Ambipolar molecules are rare, and they can enable low-power complementary-like circuits. This low band gap, asymmetric linear acene contains electron-withdrawing fluorine atoms, which lower the molecular orbital energies, allowing the injection of electrons. While hole and electron mobilities of up to 0.071 and 0.37 cm2/V.s, respectively, are reported on devices measured in nitrogen, hole mobilities of up to 0.12 cm2/V.s were found in ambient, with electron transport quenched. These devices were fabricated on octadecyltrimethoxysilane-treated surfaces at a substrate temperature of 60 degrees C.
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Various methods for the patterned assembly of metal nanoparticles have been developed in order to harness their unique electrical and optical properties for device applications. This paper discusses a method for direct writing of Au nanoparticles at nanoscale resolution using dip-pen nanolithography. First, a procedure was developed for increasing the loading of Au nanoparticles onto AFM tips to prolong patterning life. AFM tips were subsequently imaged by scanning electron microscopy to determine ink coverage and to gain insight into the deposition process. Next, surface interactions, relative humidity, and writing speed were controlled to determine an optimal range of conditions for deposition. Various ink-substrate combinations were studied to elucidate the dependence of deposition on interactions between Au nanoparticles and the substrate surface; inks consisted of positively and negatively charged particles, and substrates were SiO(2) surfaces modified as hydrophilic or hydrophobic and interacted electrostatically or covalently with Au nanoparticles. Results indicate that a highly hydrophilic surface is required for Au nanoparticle deposition, unless covalent binding can occur between the Au and substrate surface. The optimal range of relative humidity for patterning was found to be 40-60%, and Au nanoparticle deposition was not sensitive to writing speeds ranging from 0.01 to 2 microm/s.
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Cristalização/métodos , Ouro/química , Microfluídica/métodos , Microscopia de Força Atômica/métodos , Nanoestruturas/química , Nanoestruturas/ultraestrutura , Nanotecnologia/métodos , Substâncias Macromoleculares/química , Teste de Materiais , Conformação Molecular , Tamanho da Partícula , Propriedades de SuperfícieRESUMO
Processable, single-layered graphene oxide (GO) is an intriguing nanomaterial with tremendous potential for electronic applications. We spin-coated GO thin-films on quartz and characterized their sheet resistance and optical transparency using different reduction treatments. A thermal graphitization procedure was most effective, producing films with sheet resistances as low as 10(2) -10(3) Omega/square with 80% transmittance for 550 nm light. Our experiments demonstrate solution-processed GO films have potential as transparent electrodes.
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Cristalização/métodos , Grafite/química , Microeletrodos , Nanoestruturas/química , Nanoestruturas/ultraestrutura , Nanotecnologia/instrumentação , Titânio/química , Condutividade Elétrica , Desenho de Equipamento , Análise de Falha de Equipamento , Substâncias Macromoleculares/química , Teste de Materiais , Conformação Molecular , Nanotecnologia/métodos , Óxidos/química , Tamanho da Partícula , Refratometria , Soluções , Propriedades de SuperfícieRESUMO
Three-branched DNA molecules have been designed and assembled from oligonucleotide components. These nucleic acid constructs contain double- and single-stranded regions that control the hybridization behavior of the assembly. Specific localization of a single streptavidin molecule at the center of the DNA complex has been investigated as a model system for the directed placement of nanostructures. Highly selective silver and copper metallization of the DNA template has also been characterized. Specific hybridization of these DNA complexes to oligonucleotide-coupled nanostructures followed by metallization should provide a bottom-up self-assembly route for the fabrication and characterization of discrete three-terminal nanodevices.
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DNA/química , Eletrônica/métodos , Nanotecnologia/métodos , Cobre/química , DNA de Cadeia Simples/química , Microscopia de Força Atômica , Microscopia Eletrônica de TransmissãoRESUMO
DNA-based nanotechnology is a vibrant and expanding field. The specific molecular recognition properties and large aspect ratio of DNA make the molecule a promising template for bottom-up fabrication of nanowires and nanodevices. Fabricating well-defined DNA-templated nanowires requires aligned surface deposition and specific metallization of DNA molecules. DNA localization on surfaces has been achieved by bulk fluid flow or a moving air-water interface, and localization efficiency has been improved by surface modifications that favor DNA-substrate interaction. DNA-templated nanowires have been constructed from gold, silver, copper, palladium, and platinum, and template modifications have allowed the bottom-up construction of a simple electronic nanodevice. These achievements demonstrate the promising feasibility of using bottom-up nanofabrication to create increasingly sophisticated nanodevices.