10 research outputs found

    Highly Flexible MoS<sub>2</sub> Thin-Film Transistors with Ion Gel Dielectrics

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    Molybdenum disulfide (MoS<sub>2</sub>) thin-film transistors were fabricated with ion gel gate dielectrics. These thin-film transistors exhibited excellent band transport with a low threshold voltage (<1 V), high mobility (12.5 cm<sup>2</sup>/(V·s)) and a high on/off current ratio (10<sup>5</sup>). Furthermore, the MoS<sub>2</sub> transistors exhibited remarkably high mechanical flexibility, and no degradation in the electrical characteristics was observed when they were significantly bent to a curvature radius of 0.75 mm. The superior electrical performance and excellent pliability of MoS<sub>2</sub> films make them suitable for use in large-area flexible electronics

    Wood–Graphene Oxide Composite for Highly Efficient Solar Steam Generation and Desalination

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    Solar steam generation is a highly promising technology for harvesting solar energy, desalination and water purification. We introduce a novel bilayered structure composed of wood and graphene oxide (GO) for highly efficient solar steam generation. The GO layer deposited on the microporous wood provides broad optical absorption and high photothermal conversion resulting in rapid increase in the temperature at the liquid surface. On the other hand, wood serves as a thermal insulator to confine the photothermal heat to the evaporative surface and to facilitate the efficient transport of water from the bulk to the photothermally active space. Owing to the tailored bilayer structure and the optimal thermo-optical properties of the individual components, the wood–GO composite structure exhibited a solar thermal efficiency of ∌83% under simulated solar excitation at a power density of 12 kW/m<sup>2</sup>. The novel composite structure demonstrated here is highly scalable and cost-efficient, making it an attractive material for various applications involving large light absorption, photothermal conversion and heat localization

    Influence of Surface Charge of the Nanostructures on the Biocatalytic Activity

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    The physicochemical properties of abiotic nanostructures determine the structure and function of biological counterparts in biotic–abiotic nanohybrids. A comprehensive understanding of the interfacial interactions and the predictive capability of their structure and function is paramount for virtually all fields of bionanotechnology. In this study, using plasmonic nanostructures as a model abiotic system, we investigate the effect of the surface charge of nanostructures on the biocatalytic reaction kinetics of a bound enzyme. We found that the surface charge of nanostructures profoundly influences the structure, orientation, and activity of the bound enzyme. Furthermore, the interactions of the enzyme with nanoparticles result in stable conjugates that retain their functionality at elevated temperatures, unlike their free counterparts that lose their secondary structure and biocatalytic activity

    PEGylated Artificial Antibodies: Plasmonic Biosensors with Improved Selectivity

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    Molecular imprinting, which involves the formation of artificial recognition elements or cavities with complementary shape and chemical functionality to the target species, is a powerful method to overcome a number of limitations associated with natural antibodies. An important but often overlooked consideration in the design of artificial biorecognition elements based on molecular imprinting is the nonspecific binding of interfering species to noncavity regions of the imprinted polymer. Here, we demonstrate a universal method, namely, PEGylation of the noncavity regions of the imprinted polymer, to minimize the nonspecific binding and significantly enhance the selectivity of the molecular imprinted polymer for the target biomolecules. The nonspecific binding, as quantified by the localized surface plasmon resonance shift of imprinted plasmonic nanorattles upon exposure to common interfering proteins, was found to be more than 10 times lower compared to the non-PEGylated counterparts. The method demonstrated here can be broadly applied to a wide variety of functional monomers employed for molecular imprinting. The significantly higher selectivity of PEGylated molecular imprints takes biosensors based on these artificial biorecognition elements closer to real-world applications

    Plasmonic Nanogels for Unclonable Optical Tagging

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    We demonstrate the fabrication of novel functional gel coatings with randomized physical and chemical patterns that enable dual encoding ability to realize unclonable optical tags. This design is based on swelling-mediated massive reconstruction of an ultrathin responsive gelatinous polymer film uniformly adsorbed with plasmonic nanostructures into a randomized network of interacting folds, resulting in bright electromagnetic hotspots within the folds. We reveal a strong correlation between the topology and near-field electromagnetic field enhancement due to the intimate contact between two plasmonic surfaces within the folds, each of them representing a unique combination of local topography and chemical distribution caused by the formation of electromagnetic hotspots. Because of the efficient trapping of the Raman reporters within the uniquely distributed electromagnetic hotspots, the surface enhanced Raman scattering enhancement from the morphed plasmonic gel was found to be nearly 40 times higher compared to that from the pristine plasmonic gel. Harnessing the nondeterministic nature of the folds, the folded plasmonic gel can be employed as a multidimensional (with dual topo-chemical encoding) optical taggant for prospective anticounterfeiting applications. Such novel optical tags based on the spontaneous folding process are virtually impossible to replicate because of the combination of nondeterministic physical patterns and chemical encoding

    Plasmonic Biofoam: A Versatile Optically Active Material

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    Owing to their ability to confine and manipulate light at the nanoscale, plasmonic nanostructures are highly attractive for a broad range of applications. While tremendous progress has been made in the synthesis of size- and shape-controlled plasmonic nanostructures, their integration with other materials and application in solid-state is primarily through their assembly on rigid two-dimensional (2D) substrates, which limits the plasmonically active space to a few nanometers above the substrate. In this work, we demonstrate a simple method to create plasmonically active three-dimensional biofoams by integrating plasmonic nanostructures with highly porous biomaterial aerogels. We demonstrate that plasmonic biofoam is a versatile optically active platform that can be harnessed for numerous applications including (i) ultrasensitive chemical detection using surface-enhanced Raman scattering; (ii) highly efficient energy harvesting and steam generation through plasmonic photothermal heating; and (iii) optical control of enzymatic activity by triggered release of biomolecules encapsulated within the aerogel. Our results demonstrate that 3D plasmonic biofoam exhibits significantly higher sensing, photothermal, and loading efficiency compared to conventional 2D counterparts. The design principles and processing methodology of plasmonic aerogels demonstrated here can be broadly applied in the fabrication of other functional foams

    Hydrophilic, Bactericidal Nanoheater-Enabled Reverse Osmosis Membranes to Improve Fouling Resistance

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    Polyamide (PA) semipermeable membranes typically used for reverse osmosis water treatment processes are prone to fouling, which reduces the amount and quality of water produced. By synergistically coupling the photothermal and bactericidal properties of graphene oxide (GO) nanosheets, gold nanostars (AuNS), and hydrophilic polyethylene glycol (PEG) on PA reverse osmosis membrane surfaces, we have dramatically improved fouling resistance of these membranes. Batch fouling experiments from three classes of fouling are presented: mineral scaling (CaCO<sub>3</sub> and CaSO<sub>4</sub>), organic fouling (humic acid), and biofouling (<i>Escherichia coli</i>). Systematic analyses and a variety of complementary techniques were used to elucidate fouling resistance mechanisms from each layer of modification on the membrane surface. Both mineral scaling and organic fouling were significantly reduced in PA–GO–AuNS–PEG membranes compared to other membranes. The PA–GO–AuNS–PEG membrane was also effective in killing all near-surface bacteria compared to PA membranes. In the PA–GO–AuNS–PEG membrane, the GO nanosheets act as templates for <i>in situ</i> AuNS growth, which then facilitated localized heating upon irradiation by an 808 nm laser inactivating bacteria on the membrane surface. Furthermore, AuNS in the membrane assisted PEG in preventing mineral scaling on the membrane surface. In flow-through flux and foulant rejection tests, PA–GO–AuNS–PEG membranes performed better than PA membranes in the presence of CaSO<sub>4</sub> and humic acid model foulants. Therefore, the newly suggested membrane surface modifications will not only reduce fouling from RO feeds, but can improve overall membrane performance. Our innovative membrane design reported in this study can significantly extend the lifetime and water treatment efficacy of reverse osmosis membranes to alleviate escalating global water shortage from rising energy demands

    Silk-Encapsulated Plasmonic Biochips with Enhanced Thermal Stability

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    Because of their high sensitivity, cost-efficiency, and great potential as point-of-care biodiagnostic devices, plasmonic biosensors based on localized surface plasmon resonance have gained immense attention. However, most plasmonic biosensors and conventional bioassays rely on natural antibodies, which are susceptible to elevated temperatures and nonaqueous media. Hence, an expensive and cumbersome “cold chain” system is necessary to preserve the labile antibodies by maintaining optimal cold temperatures during transport, storage, and handling. Herein, we introduce a facile approach to preserve the antibody activity on a biosensor surface even at elevated temperatures. We show that silk fibroin film could be used as a protective layer to preserve the activity of a model antibody (Rabbit IgG) and cardiac troponin antibody at both room temperature and 40 °C over several days. Furthermore, a simple aqueous rinsing process restores the biofunctionality of the biosensor. This energy-efficient and environmentally friendly method represents a novel approach to eliminate the cold chain and temperature-controlled packing of diagnostic reagents and materials, thereby extending the capability of antibody-based biosensors to different resource-limited circumstances such as developing countries, an ambulance, an intensive care unit emergency room, and battlefield

    Graphene-Based High-Efficiency Surface-Enhanced Raman Scattering-Active Platform for Sensitive and Multiplex DNA Detection

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    We have developed a surface-enhanced Raman scattering (SERS)-active substrate based on gold nanoparticle-decorated chemical vapor deposition (CVD)-growth graphene and used it for multiplexing detection of DNA. Due to the combination of gold nanoparticles and graphene, the Raman signals of dye were dramatically enhanced by this novel substrate. With the gold nanoparticles, DNA capture probes could be easily assembled on the surface of graphene films which have a drawback to directly immobilize DNA. This platform exhibits extraordinarily high sensitivity and excellent specificity for DNA detection. A detection limit as low as 10 pM is obtained. Importantly, two different DNA targets could be detected simultaneously on the same substrate just using one light source

    Growth of Large-Area and Highly Crystalline MoS<sub>2</sub> Thin Layers on Insulating Substrates

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    The two-dimensional layer of molybdenum disulfide (MoS<sub>2</sub>) has recently attracted much interest due to its direct-gap property and potential applications in optoelectronics and energy harvesting. However, the synthetic approach to obtain high-quality and large-area MoS<sub>2</sub> atomic thin layers is still rare. Here we report that the high-temperature annealing of a thermally decomposed ammonium thiomolybdate layer in the presence of sulfur can produce large-area MoS<sub>2</sub> thin layers with superior electrical performance on insulating substrates. Spectroscopic and microscopic results reveal that the synthesized MoS<sub>2</sub> sheets are highly crystalline. The electron mobility of the bottom-gate transistor devices made of the synthesized MoS<sub>2</sub> layer is comparable with those of the micromechanically exfoliated thin sheets from MoS<sub>2</sub> crystals. This synthetic approach is simple, scalable, and applicable to other transition metal dichalcogenides. Meanwhile, the obtained MoS<sub>2</sub> films are transferable to arbitrary substrates, providing great opportunities to make layered composites by stacking various atomically thin layers
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