Nanoribbon Yarn with Versatile Inorganic Materials.

Nanomaterial-based yarns have been actively developed owing to their advantageous features, namely, high surface-area-to-volume ratios, flexibility, and unusual material characteristics such as anisotropy in electrical/thermal conductivity. The superior properties of the nanomaterials can be directly imparted and scaled-up to macro-sized structures. However, most nanomaterial-based yarns have thus far, been fabricated with only organic materials such as polymers, graphene, and carbon nanotubes. This paper presents a novel fabrication method for fully inorganic nanoribbon yarn, expanding its applicability by bundling highly aligned and suspended nanoribbons made from various inorganic materials (e.g., Au, Pd, Ni, Al, Pt, WO3, SnO2, NiO, In2O3, and CuO). The process involves depositing the target inorganic material on a nanoline mold, followed by suspension through plasma etching of the nanoline mold, and twisting using a custom-built yarning machine. Nanoribbon yarn structures of various functional inorganic materials are utilized for chemical sensors (Pd-based H2 and metal oxides (MOx)-based green gas sensors) and green energy transducers (water splitting electrodes/triboelectric nanogenerators). This method is expected to provide a comprehensive fabrication strategy for versatile inorganic nanomaterials-based yarns.

Plasmonic color filters fabricated via oxide-based nanotransfer printing.

Plasmonic filters have recently become a topic of significant interest because they are suitable for a wide range of applications. However, effective fabrication of plasmonic filters remains a challenge. In this paper, we demonstrate a simple method for fabricating plasmonic color filters based on nanotransfer printing (nTP) , using SiO2 as a hard mask for Al etching. nTP was performed on a 100 nm Al layer deposited on a glass wafer substrate with a 10 nm Al layer and a 20 nm SiO2 layer with a nanohole pattern. The 10 nm Al layer and 20 nm SiO2 layers were previously transferred from a polymer stamp prepared to create patterns of subwavelength-sized holes. The plasmonic filters were ultimately fabricated using the SiO2 layer as a hard mask to selectively etch the Al layer. The optical properties of the fabricated plasmonic filters were evaluated using experimental and simulation tools. In addition, we analyzed the results of nTP on the Al and SiO2 films by varying the temperature, pressure, and SiO2-film thickness. We believe that this technique is a promising method for fabricating nanostructures and for widening the scope of practical application of plasmonics because of its high efficiency and cost-effectiveness.

Illuminating Recent Progress in Nanotransfer Printing: Core Principles, Emerging Applications, and Future Perspectives.

As the demand for diverse nanostructures in physical/chemical devices continues to rise, the development of nanotransfer printing (nTP) technology is receiving significant attention due to its exceptional throughput and ease of use. Over the past decade, researchers have attempted to enhance the diversity of materials and substrates used in transfer processes as well as to improve the resolution, reliability, and scalability of nTP. Recent research on nTP has made continuous progress, particularly using the control of the interfacial adhesion force between the donor mold, target material, and receiver substrate, and numerous practical nTP methods with niche applications have been demonstrated. This review article offers a comprehensive analysis of the chronological advancements in nTP technology and categorizes recent strategies targeted for high-yield and versatile printing based on controlling the relative adhesion force depending on interfacial layers. In detail, the advantages and challenges of various nTP approaches are discussed based on their working mechanisms, and several promising solutions to improve morphological/material diversity are presented. Furthermore, this review provides a summary of potential applications of nanostructured devices, along with perspectives on the outlook and remaining challenges, which are expected to facilitate the continued progress of nTP technology and to inspire future innovations.

Nanoscale three-dimensional fabrication based on mechanically guided assembly.

The growing demand for complex three-dimensional (3D) micro-/nanostructures has inspired the development of the corresponding manufacturing techniques. Among these techniques, 3D fabrication based on mechanically guided assembly offers the advantages of broad material compatibility, high designability, and structural reversibility under strain but is not applicable for nanoscale device printing because of the bottleneck at nanofabrication and design technique. Herein, a configuration-designable nanoscale 3D fabrication is suggested through a robust nanotransfer methodology and design of substrate's mechanical characteristics. Covalent bonding-based two-dimensional nanotransfer allowing for nanostructure printing on elastomer substrates is used to address fabrication problems, while the feasibility of configuration design through the modulation of substrate's mechanical characteristics is examined using analytical calculations and numerical simulations, allowing printing of various 3D nanostructures. The printed nanostructures exhibit strain-independent electrical properties and are therefore used to fabricate stretchable H2 and NO2 sensors with high performances stable under external strains of 30%.

Nanotransfer-on-Things: From Rigid to Stretchable Nanophotonic Devices.

The growing demand for nanophotonic devices has driven the advancement of nanotransfer printing (nTP) technology. Currently, the scope of nTP is limited to certain materials and substrates owing to the temperature, pressure, and chemical bonding requirements. In this study, we developed a universal nTP technique utilizing covalent bonding-based adhesives to improve the adhesion between the target material and substrate. Additionally, the technique employed plasma-based selective etching to weaken the adhesion between the mold and target material, thereby enabling the reliable modulation of the relative adhesion forces, regardless of the material or substrate. The technique was evaluated by printing four optical materials on nine substrates, including rigid, flexible, and stretchable substrates. Finally, its applicability was demonstrated by fabricating a ring hologram, a flexible plasmonic color filter, and extraordinary optical transmission-based strain sensors. The high accuracy and reliability of the proposed nTP method were verified by the performance of nanophotonic devices that closely matched numerical simulation results.

Recent Advances in Sensor-Actuator Hybrid Soft Systems: Core Advantages, Intelligent Applications, and Future Perspectives.

The growing demand for soft intelligent systems, which have the potential to be used in a variety of fields such as wearable technology and human-robot interaction systems, has spurred the development of advanced soft transducers. Among soft systems, sensor-actuator hybrid systems are considered the most promising due to their effective and efficient performance, resulting from the synergistic and complementary interaction between their sensor and actuator components. Recent research on integrated sensor and actuator systems has resulted in a range of conceptual and practical soft systems. This review article provides a comprehensive analysis of recent advances in sensor and actuator integrated systems, which are grouped into three categories based on their primary functions: i) actuator-assisted sensors for intelligent detection, ii) sensor-assisted actuators for intelligent movement, and iii) sensor-actuator interactive devices for a hybrid of intelligent detection and movement. In addition, several bottlenecks in current studies are discussed, and prospective outlooks, including potential applications, are presented. This categorization and analysis will pave the way for the advancement and commercialization of sensor and actuator-integrated systems.

Functional Asymmetry-Enabled Self-Adhesive Film via Phase Separation of Binary Polymer Mixtures for Soft Bio-Integrated Electronics.

Biocompatible adhesive films are important for many applications (e.g., wearable devices, implantable devices, and attachable sensors). In particular, achieving self-adhesion on one side of a film with biocompatible materials is a compelling goal in adhesion science. Herein, we report a simple and easy manufacturing process using water-soluble hyaluronic acid (HA) that allows adhesiveness on only one side using binary polymer mixtures based on a phase-separation strategy with an elastomer. HA influx allows for the entangled polymer chains of the elastomer to spontaneously deform, permitting tunable mechanical elasticity, conformability, and adhesion. The proposed adhesive film enables the transfer of nanopatterning and the attachment of various surfaces without the use of additional chemicals. In addition, the film can be used for measuring epidermal biopotential and for skin fixation of drug devices. Therefore, the developed facile asymmetric adhesion can block the interferences of other materials on the unnecessary adhesion side, providing considerable potential for the development of functional, multifunctional, and smart bioadhesives.

Biocompatible All-in-One Adhesive Needle-Free Cup Patch for Enhancing Transdermal Drug Delivery.

Patch-type drug delivery has garnered increased attention as an attractive alternative to the existing drug delivery techniques. Thus far, needle phobia and efficient drug delivery remain huge challenges. To address the issue of needle phobia and enhance drug delivery, we developed a needle-free and self-adhesive microcup patch that can be loaded with an ultrathin salmon DNA (SDNA) drug carrier film. This physically integrated system can facilitate efficient skin penetration of drugs loaded into the microcup patch. The system consists of three main components, namely, a cup that acts as a drug reservoir, an adhesive system that attaches the patch to the skin, and physical stimulants that can be used to increase the efficiency of drug delivery. In addition, an ultrathin SDNA/drug film allows the retention of the drug in the cup and its efficient release by dissolution in the presence of moisture. This latter feature has been validated using gelatin as a skin mimic. The cup design itself has been validated by comparing its deformation and displacement with those of a cylindrical structure. Integration of the self-adhesive microcup patch with both ultrasonic waves and an electric current allows the model drug to penetrate the stratum corneum of the skin barrier and the whole epidermis, thereby enhancing transdermal drug delivery and reducing skin irritation. This system can be used as a wearable biomedical device for efficient transdermal and needle-free drug delivery.

Shape-Controlled and Well-Arrayed Heterogeneous Nanostructures via Melting Point Modulation at the Nanoscale.

A novel method for fabricating shape-controlled and well-arrayed heterogeneous nanostructures by altering the melting point of the metal thin film at the nanoscale is proposed. Silver nanofilms (AgNFs) are transformed into silver nanoislands (AgNIs), silver nanoparticles (AgNPs), and silver nanogaps (AgNGs) that are well-ordered and repositioned inside the gold nanoholes (AuNHs) depending on the diameter of the AuNHs, the thickness of the AgNF, and the heating temperature (120-200 °C). This method demonstrates the ability to fabricate uniform, stable, and unique structures with a fast, simple, and mass-producible process. For demonstrating the diverse applicability of the developed structures, high-density AgNGs inside the AuNHs are utilized as surface-enhanced Raman spectroscopy (SERS) substrates. These AgNGs-based SERS substrates exhibit a performance enhancement, which is 1.06 × 106 times greater than that of a metal film, with a relative standard deviation of 19.8%. The developed AgNP/AgNI structures are also used as nonreproducible anti-counterfeiting signs, and the anti-counterfeiting/readout system is demonstrated via image processing. Therefore, our method could play a vital role in the nanofabrication of high-demand nanostructures.

Biocompatible Nanotransfer Printing Based on Water Bridge Formation in Hyaluronic Acid and Its Application to Smart Contact Lenses.

Many conventional micropatterning and nanopatterning techniques employ toxic chemicals, rendering them nonbiocompatible and unsuited for biodevice production. Herein the formation of water bridges on the surface of hyaluronic acid (HA) films is exploited to develop a transfer-based nanopatterning method applicable to diverse structures and materials. The HA film surface, made deformable via water bridge generation, is brought into contact with a functional material and subjected to thermal treatment, which results in film shrinkage, allowing a robust pattern transfer. The proposed biocompatible method, which avoids the use of extra chemicals, enables the transfer of nanoscale, microscale, and thin-film structures as well as functional materials such as metals and metal oxides. A nanopatterned HA film is transferred onto a moisture-containing contact lens to fabricate smart contact lenses with unique optical characteristics of rationally designed optical nanopatterns. These lenses demonstrated binocular parallax-induced stereoscopy via nanoline array polarization and acted as cutoff filters, with nanodot arrays, capable of treating Irlen syndrome.

Large-Area Nanogap-Controlled 3D Nanoarchitectures Fabricated via Layer-by-Layer Nanoimprint.

The fabrication of large-area and flexible nanostructures currently presents various challenges related to the special requirements for 3D multilayer nanostructures, ultrasmall nanogaps, and size-controlled nanomeshes. To overcome these rigorous challenges, a simple method for fabricating wafer-scale, ultrasmall nanogaps on a flexible substrate using a temperature above the glass transition temperature (Tg) of the substrate and by layer-by-layer nanoimprinting is proposed here. The size of the nanogaps can be easily controlled by adjusting the pressure, heating time, and heating temperature. In addition, 3D multilayer nanostructures and nanocomposites with 2, 3, 5, 7, and 20 layers were fabricated using this method. The fabricated nanogaps with sizes ranging from approximately 1 to 40 nm were observed via high-resolution transmission electron microscopy (HRTEM). The multilayered nanostructures were evaluated using focused ion beam (FIB) technology. Compared with conventional methods, our method could not only easily control the size of the nanogaps on the flexible large-area substrate but could also achieve fast, simple, and cost-effective fabrication of 3D multilayer nanostructures and nanocomposites without any post-treatment. Moreover, a transparent electrode and nanoheater were fabricated and evaluated. Finally, surface-enhanced Raman scattering substrates with different nanogaps were evaluated using rhodamine 6G. In conclusion, it is believed that the proposed method can solve the problems related to the high requirements of nanofabrication and can be applied in the detection of small molecules and for manufacturing flexible electronics and soft actuators.

Effective Dispensing Methods for Loading Drugs Only to the Tip of DNA Microneedles.

Here, we propose a novel and simple method to efficiently capture the diffusion of fluorescein isothiocyanate (FITC)-dextran from a biocompatible substance and load the drug only to the tip of DNA microneedles. A dispensing and suction method was chosen to fabricate the designed microneedles with efficient amounts of FITC as the drug model. Importantly, the vacuum process, which could influence the capturing of FITC diffusion from the tip, was evaluated during the manufacturing process. In addition, the simulations were consistent with the experimental results and showed apparent diffusion. Moreover, dextrans of different molecular weights labeled with FITC were chosen to fabricate the tip of microneedles for demonstrating their applicability. Finally, a micro-jetting system with a micro-nozzle (diameter: 80 µm) was developed to achieve the accurate and rapid loading of small amounts of FITC using the anti-diffusion and micro-jetting methods. Our method not only uses a simple and fast manufacturing process, but also fabricates the tips of microneedles more efficiently with FITC compared with the existing methods. We believe that the proposed method is essential for the clinical applications of the microneedle drug delivery platform.

3D Layer-By-Layer Pd-Containing Nanocomposite Platforms for Enhancing the Performance of Hydrogen Sensors.

Herein, a nanowelding technique is adopted to fabricate three-dimensional layer-by-layer Pd-containing nanocomposite structures with special properties. Nanowires fabricated from noble metals (Pd, Pt, Au, and Ag) were used to prepare Pd-Pd nanostructures and Pd-Au, Pd-Pt, Pd-Ag, and Pd-Pt-Au nanocomposite structures by controlling the welding temperature. The recrystallization behavior of the welded composite materials was observed and analyzed. In addition, their excellent mechanical and electrical properties were confirmed by performing 10,000 bending test cycles and measuring the resistances. Finally, flexible and wearable nanoheaters and gas sensors were fabricated using our proposed method. In comparison with conventional techniques, our proposed method can not only easily achieve sensors with a large surface area and flexibility but also improve their performance through the addition of catalyst metals. A gas sensor fabricated using the Pd-Au nanocomposites demonstrated 3.9-fold and 1.1-fold faster H2 recovery and response, respectively, than a pure Pd-Pd gas sensor device. Moreover, the Pd-Ag nanocomposite exhibited a high sensitivity of 5.5% (better than that of other fabricated gas sensors) for 1.6% H2 concentration. Therefore, we believe that the fabricated nanocomposites appear promising for wide applications in wearable gas sensors, flexible optical devices, and flexible catalytic devices.

Nanotransfer Printing on Textile Substrate with Water-Soluble Polymer Nanotemplate.

The growing interest in wearable devices has drawn increased attention to smart textiles, and various transfer methods have therefore been introduced to realize the desired functions using textiles as substrates. However, the existing transfer techniques are not suited for the production of sophisticated nanoscale patterns on textiles, as textile roughness and difficulty of precise pattern size control hinder miniaturization, deteriorate device performance, and complicate the use of optical phenomena such as surface plasmon resonance. To address these limitations, we have developed a method based on simple dissolution of a water-soluble nanopatterned polymer film for the facile transfer of nanostructures of on-film-deposited functional materials onto textile substrates. The above method tolerates a variety of functional materials, e.g., metals and SiO2, and nano/microscale structures, e.g., nanoscale lines, dots, holes, and mesh patterns with a minimum pattern width of 50 nm. The proposed technique is employed to fabricate a palladium nanoscale line array (utilized as a highly sensitive and selective hydrogen sensor) and is shown to be suitable for the production of security patterns on textiles, as it allows the printing of complex nanostructure patterns with electrical and optical functionalities.

Adhesive-Layer-Free and Double-Faced Nanotransfer Lithography for a Flexible Large-Area MetaSurface Hologram.

Herein, we develop an adhesive-free double-faced nanotransfer lithography (ADNT) technique based on the surface deformation of flexible substrates under the conditions of temperature and pressure control and thus address the challenge of realizing the mass production of large-area nanodevices in the fields of optics, metasurfaces, and holograms. During ADNT, which is conducted on a flexible polymer substrate above its glass transition temperature in the absence of adhesive materials and chemical bonding agents, nanostructures from the polymer stamp are attached to the deformed polymer substrate. Various silicon masters are employed to prove our method applicable to arbitrary nanopatterns, and diverse Ag and Au nanostructures are deposited on polymer molds to demonstrate the wide scope of useable metals. Finally, ADNT is used to (i) produce a flexible large-area hologram on the defect-free poly(methyl methacrylate) (PMMA) film and (ii) fabricate a metasurface hologram and a color filter on the front and back surfaces of the PMMA film, respectively, to realize dual functionality. Thus, it is concluded that the use of ADNT can decrease the fabrication time and cost of high-density nanodevices and facilitate their commercialization.

Repeatable and metal-independent nanotransfer printing based on metal oxidation for plasmonic color filters.

Many recently developed nanotransfer printing techniques have received much attention because of their simplicity and low cost. In addition, such techniques are suitable for fabricating nano/microscale sensors, optical elements, and electrical devices. However, conventional nanotransfer printing methods are time-consuming, cannot be easily used over large areas or with several different materials, and are not suitable for repeatedly transferring various materials onto the same substrate or a curved surface. Herein, a new nanotransfer printing method is introduced based on the oxidation of various metals and the formation of covalent bonds between spin- and spray-coatable adhesives and the chosen metal at low temperatures. These strong covalent bonds allow the fast transfer of the deposited materials from a polymer stamp without additional processing. A major advantage of this process is that it is metal-independent; nanowires of various metals are successfully transferred from the polymer stamp because strong covalent bonds form instantaneously between the metal and an adhesive-coated substrate. Moreover, this nanotransfer process can be used repeatedly to fabricate large-scale color filters from smaller areas of nanowires, regardless of the metal type and nanostructure orientation. Furthermore, plasmonic color filters composed of nanohole arrays can be obtained on both flat and curved surfaces.

Gold-Nanocluster-Assisted Nanotransfer Printing Method for Metasurface Hologram Fabrication.

Given the development of nano/microscale patterning techniques, efforts are being made to use them for fabricating metasurfaces. In particular, by using abrupt phase discontinuities, it is possible to generate holographic images from two-dimensional nanoscale-patterned metasurfaces. However, the fabrication of metasurface holograms is hindered by the high costs and long fabrication time involved, because the process requires expensive equipment such as that for electron-beam lithography. Therefore, it is difficult to realize metasurface holograms in a fast and repetitive manner. In this study, we propose a method for fabricating metasurface holograms based on the nanotransfer printing of the desired nanoscale patterns, which is assisted by Au nanoclusters, while controlling the bonding energy based on the shape of the deposited Au layer. Robust covalent bonds are formed between the Si of the adhesive used and the O of the SiO2 layer in order to transfer the deposited Au onto the transparent substrate quickly. It was found that the fabricated metasurface hologram coincides with the one designed by computer-generated holography. The proposed method should lead to a significant breakthrough in the fabrication of holograms based on different types of metasurfaces at a low cost in a fast, repetitive manner with various metals.

Microneedles integrated with a triboelectric nanogenerator: an electrically active drug delivery system.

In this study, a combined system of microneedles and a triboelectric nanogenerator (TENG) has been developed for drug delivery. A triboelectric device, which converts mechanical energy into alternating current (AC), was chosen to replace the electrophoresis (EP) effect. To directly generate triboelectricity from salmon deoxyribonucleic acid (SDNA)-based microneedles, a triboelectric series of SDNA film and chargeable polymers (polyimide and Teflon) was studied. The electrical output of the two charged polymers was compared to find a material that could be highly charged with SDNA. The electrical output was also compared as a function of the concentration of a drug embedded in the SDNA film, and the results confirmed that drug intercalation affected the carrier diffusion. The mechanical strength of the microneedles was assessed by histological analysis of their penetration into porcine cadaver skin. Furthermore, the output voltage of a system incorporating microneedles and TENG in cadaver skin, and in vitro drug release into gelatin were evaluated to examine potential application as an electrically active drug delivery system. The electrical output voltage of this system was ∼95 V. The mechanism of triboelectric perturbation to the skin has also been discussed. The system developed in this work is a new, facile approach toward effective drug delivery that replaces the existing EP method and expands the application of TENGs.

Flexible Plasmonic Color Filters Fabricated via Nanotransfer Printing with Nanoimprint-Based Planarization.

We investigated the preparation and performance of large-area transmission-type flexible plasmonic color filters (PCFs). These large-area PCFs were fabricated based on a nanotransfer printing (nTP) process that involves nanoimprint-based planarization. This process is a simple surface treatment for easy transfer of a metal to a flexible plastic substrate and formation of patterned aluminum nanodots and nanoholes on a substrate surface with poor roughness. Rabbit-ear structures can form during the nTP process, and this phenomenon was analyzed by numerical simulation. As defects were not detected in a 10 000-round bending test, the PCFs fabricated using this nTP process have excellent mechanical properties.

Three-dimensional plasmonic Ag/TiO2 nanocomposite architectures on flexible substrates for visible-light photocatalytic activity.

In this study, a periodic three-dimensional (3D) Ag/TiO2 nanocomposite architecture of nanowires was fabricated on a flexible substrate to enhance the plasmonic photocatalytic activity of the composite. Layer-by-layer nanofabrication based on nanoimprint lithography, vertical e-beam evaporation, nanotransfer, and nanowelding was applied in a new method to create different 3D Ag/TiO2 nanocomposite architectures. The fabricated samples were characterized by scanning electron microscopy, transmission electron microscopy, focused ion-beam imaging, X-ray photoelectron spectrometry, and UV-visible spectroscopy. The experiment indicated that the 3D nanocomposite architectures could effectively enhance photocatalytic activity in the degradation of methylene blue solution under visible light irradiation. We believe that our method is efficient and stable, which could be applied to various fields, including photocatalysis, solar energy conversion, and biotechnology.