Experimental validation for the interconversion between generalized Kelvin-Voigt and Maxwell models using human skin tissues.

Mechanical properties of biological systems provide essential insights into their component, physiological function, and disease mechanism under various conditions, such as age, health, and other environmental factors. Viscoelasticity is one of the most important and investigated properties to study biomaterials, cells, and tissues, as they exhibit the characteristics of both fluid-like behavior, viscosity, and solid-like behavior, elasticity. Various mathematical models, such as the Kelvin-Voigt and Maxwell models, have been developed and practiced to estimate and extract viscoelastic properties. However, one of the inherent challenges with the use of these models is the poor transferability of mathematically estimated viscoelastic properties across different models, largely due to variations in constituent elements and their arrangements within each model. This issue impedes the interconversion of parameters of one model to another and complicates comparison across models. In this study, we demonstrate the equivalence between the generalized Maxwell and generalized Kelvin-Voigt models through two distinct approaches: indirect, Maxwell model-based Kelvin-Voigt model estimation and direct, curve fitting-based Kelvin-Voigt model estimation. We utilized human melanoma skin tissues to estimate viscoelastic properties using the Prony series. The estimated parameters and resulting viscoelastic properties revealed no significant difference between the two approaches and between the two patients. This study is the first experimental validation of the mathematical interconversion of the two models, signifying that this approach will enable an accurate and objective analysis and comparison of mechanical properties across various viscoelastic models.

Cost-Effective and Facile Fabrication of a Tattoo Paper-Based SERS Substrate and Its Application in Pesticide Sensing on Fruit Surfaces.

Surface-enhanced Raman spectroscopy (SERS) has been transformed into a useful analytical technique with significant advantages in relation to sensitive and low-concentration chemical analyses. However, SERS substrates are expensive and the analyte sample preparation is complicated; hence, it is only used in limited areas. We have fabricated a tattoo paper-based SERS substrate by using non-complicated inkjet printing. The sensitivity of the SERS substrate was increased by removing the carbon residues via exposure to ultraviolet light without damaging the substrate. Thus, low concentrations of pesticides (up to 1 µM thiram) were measured. The SERS substrate was attached to the curved surface of an apple to demonstrate its advantages, such as the flexibility and easy attachability of tattoo paper, and its feasibility was verified by measuring 1 µM thiram on the apple's surface. Due to its economic cost, simple usage, and rapid measurement, it will be helpful for the identification of both agricultural adulterants and food adulterants and for water-based pollutant detection. It will also possibly be helpful for medical purposes related to human body surfaces in the future.

Experimental Study on Ion Transport in Microfluidic Electrodialysis Using Partially Masked Ion Exchange Membranes.

Electrodialysis using anion-exchange membranes (AEMs) and cation-exchange membranes (CEMs) has been widely used for water desalination and the management of various ionic species. During commercial electrodialysis, the available area of an ion-exchange membrane is reduced by a non-conductive spacer that is in contact with the AEM/CEM. Although multiple reports have described the advantages or disadvantages of spacers, fewer studies have explored the effects of spacers on the mass transport effect of the reduced membrane area excluding the fluid flow change. In this paper, we present our experimental studies concerning mass transport in microfluidic electrodialysis systems with partially masked ion-exchange membranes. Six different types of masking membranes were prepared by the deposition of non-conductive films on parts of the membranes. The experimental results showed that the overlapped types (in which masking was vertically aligned in the AEM/CEM) exhibited a larger electrical conductance and better current/energy efficiency, compared with the non-overlapped types (in which masking was vertically dislocated in the AEM/CEM). We also observed that a reduction in the unit length of the unmasked ion-exchange membrane enhanced overall mass transport. Our results demonstrate the effects of patterned membranes on electrical resistance and desalination performance; they also identify appropriate arrangements for electromembrane systems.

Design of Large-Scale Microwave Cavity for Uniform and Efficient Plastic Heating.

To reduce carbon emissions during heating in the manufacturing processes, microwave technology has attracted significant attention. Microwaves have considerable advantages over traditional heating methods, including more rapid heating, lower thermal damage, and eco-friendly processes. To apply microwaves to the manufacturing process, uniform and efficient heating is required. We analyzed the effect of various design parameters for uniform and efficient heating by changing the cavity heights, application of the reflector, and number and positions of waveguides. We conducted a numerical simulation and verified the findings by experiments. The results showed that a slight change in the cavity height altered the electromagnetic field distribution and heating parameters, such as the coefficient of variance and power absorption efficiency. With reflectors installed, 66% of cases exhibited better comprehensive evaluation coefficient (CEC) with consideration of uniform heating and power absorption. The spherical reflector showed 81% of cases, better than those of the ordinary model without a reflector. Furthermore, when double waveguides were installed, the average coefficient of variance (COV) was improved by 22%, and power absorption efficiency was increased by 53% compared to the single waveguide case. When the power applied to the waveguides was doubled, the average COV values improved by 18%. This large-scale analysis will be helpful in applying microwaves to actual industrial sites.

Nanogap Formation Using a Chromium Oxide Film and Its Application as a Palladium Hydrogen Switch.

Developing high response hydrogen sensors manufacturable in a large scale is desirable in hydrogen industry. In this study, a chromium oxidation-based nanogap formation process was developed to fabricate a hydrogen switch with suspended palladium and gold films having a tens of nanometer-sized gap. The nanogap was formed by using oxidized chromium as a self-alignment shadow mask. The hydrogen switch operates by the principle of volume expansion of palladium upon exposure to the hydrogen gas and the current reading by closing of a nanogap formed between suspended palladium and gold films. Further improvement of the sensor performance was achieved by optimizing the design parameters such as suspended film lengths and thicknesses. The fabricated palladium nanogap hydrogen sensor showed an ultrahigh sensitivity of ΔI/I0 > 108 with a fast response time (22 s) to 4% hydrogen. The complementary metal-oxide-semiconductor-compatible fabrication of the hydrogen switch is easily scalable with low manufacturing cost.

Self-Powered Gas Sensor Based on a Photovoltaic Cell and a Colorimetric Film with Hierarchical Micro/Nanostructures.

We report a new type of self-powered gas sensors based on the combination of a colorimetric film with hierarchical micro/nanostructures and organic photovoltaic cells. The transmittance of the colorimetric film with micro/nanostructures coated with N,N,N',N'-tetramethyl-p-phenylenediamine (TMPD) changes by reacting with NO2 gas, and it is measured as a current output of the photovoltaic cell. For this purpose, materials for the organic photovoltaic cells were carefully chosen to match the working wavelength of the TMPD. Micropost arrays and nanowires increase the surface area for the gas reaction and thus improve the transmittance changes by NO2 gas (6.7% change for the plain film vs 27.7% change for the film with hierarchical micro/nanostructures to 20 ppm of NO2). Accordingly, the colorimetric device with the hierarchical structures showed a response of ΔI/I0 = 0.27-20 ppm of NO2, which is a 71% improvement compared to that of the plain sensing film. Furthermore, it showed a high selectivity against other gases such as H2S and CO with almost negligible responses. Since the current output change of the photovoltaic cell is utilized as a sensor signal, no extra electrical power is required for the operation of gas sensors. We also integrated the sensor device with an electrical module and demonstrated a self-powered gas alarm system.

Overcoming evanescent field decay using 3D-tapered nanocavities for on-chip targeted molecular analysis.

Enhancement of optical emission on plasmonic nanostructures is intrinsically limited by the distance between the emitter and nanostructure surface, owing to a tightly-confined and exponentially-decaying electromagnetic field. This fundamental limitation prevents efficient application of plasmonic fluorescence enhancement for diversely-sized molecular assemblies. We demonstrate a three-dimensionally-tapered gap plasmon nanocavity that overcomes this fundamental limitation through near-homogeneous yet powerful volumetric confinement of electromagnetic field inside an open-access nanotip. The 3D-tapered device provides fluorescence enhancement factors close to 2200 uniformly for various molecular assemblies ranging from few angstroms to 20 nanometers in size. Furthermore, our nanostructure allows detection of low concentration (10 pM) biomarkers as well as specific capture of single antibody molecules at the nanocavity tip for high resolution molecular binding analysis. Overcoming molecule position-derived large variations in plasmonic enhancement can propel widespread application of this technique for sensitive detection and analysis of complex molecular assemblies at or near single molecule resolution.

Gas Sensor by Direct Growth and Functionalization of Metal Oxide/Metal Sulfide Core-Shell Nanowires on Flexible Substrates.

We have developed a novel fabrication method for flexible gas sensors for toxic gases based on sequential wet chemical reaction. In specific, zinc oxide (ZnO) nanowires were locally synthesized and directly integrated on a flexible polymer substrate using localized hydrothermal synthesis methods and their surfaces were selectively functionalized with palladium (Pd) nanoparticles using a liquid phase deposition process. Because the entire process is conducted at a low temperature in a mild precursor solution, it can be applied for flexible substrates. Furthermore, the surface of ZnO nanowires was sulfurized by hydrogen sulfide (H2S) gas to form zinc oxide/zinc sulfide (ZnO/ZnS) core-shell nanowires for stable sensing of H2S gas. The locally synthesized ZnO/ZnS core-shell nanowires enable an ultracompact-sized device, and Pd nanoparticles improve the sensing performance and reduce the operating temperature (200 °C). The device shows a high sensitivity [(Ggas - Gair)/Gair × 100% = 4491% to 10 ppm], fast response (response/recovery time <100 s) to hydrogen sulfide, and outstanding selectivity (>100 times) to other toxic gases (e.g., carbon monoxide, acetone, ethanol, and toluene). Moreover, vertically synthesized nanowires provide a long bending path, which reduces the mechanical stresses on the structure. The devices showed stable gas sensing performance under 9 mm positive radius of curvature and 5 mm negative radius of curvature. The mechanical robustness of the device was also verified by numerical simulations which showed dramatic decrease of maximum stress and strain to 4.2 and 5.0%, respectively.

Glucose Sensing Using Surface-Enhanced Raman-Mode Constraining.

Diabetes mellitus is a chronic disease, and its management focuses on monitoring and lowering a patient's glucose level to prevent further complications. By tracking the glucose-induced shift in the surface-enhanced Raman-scattering (SERS) emission of mercaptophenylboronic acid (MPBA), we have demonstrated fast and continuous glucose sensing in the physiologically relevant range from 0.1 to 30 mM and verified the underlying mechanism using numerical simulations. Bonding of glucose to MPBA suppresses the "breathing" mode of MPBA at 1071 cm-1 and energizes the constrained-bending mode at 1084 cm-1, causing the dominant peak to shift from 1071 to 1084 cm-1. MPBA-glucose bonding is also reversible, allowing continuous tracking of ambient glucose concentrations, and the MPBA-coated substrates showed very stable performance over a 30 day period, making the approach promising for long-term continuous glucose monitoring. Using Raman-mode-constrained, miniaturized SERS implants, we also successfully demonstrated intraocular glucose measurements in six ex vivo rabbit eyes within ±0.5 mM of readings obtained using a commercial glucose sensor.

Flexible Ultraviolet and Ambient Light Sensor Based on a Nanomaterial Network Fabricated Using Selective and Localized Wet Chemical Reactions.

We report ZnO nanowire- and TiO2 nanotube-based light sensors on flexible polymer substrates fabricated by localized hydrothermal synthesis and liquid phase deposition (LPD). This method realized simple and cost-effective in situ synthesis and integration of one-dimensional ZnO and TiO2 nanomaterials. The fabricated sensor devices with ZnO nanowires and TiO2 nanotubes show very high sensitivity and quick response to the ultraviolet (UV) and ambient light, respectively. In addition, our direct synthesis and integration method result in mechanical robustness under external loading such as static and cyclic bending because of the strong bonding between the nanomaterial and the electrode. By controlling the reaction time of the LPD process, the Ti/Zn ratio could be simply modulated and the spectral sensitivity to the light in the UV to visible range could be controlled.

Surface-Enhanced Raman Spectroscopy-Based Label-Free Insulin Detection at Physiological Concentrations for Analysis of Islet Performance.

Label-free optical detection of insulin would allow in vitro assessment of pancreatic cell functions in their natural state and expedite diabetes-related clinical research and treatment; however, no existing method has met these criteria at physiological concentrations. Using spatially uniform 3D gold-nanoparticle sensors, we have demonstrated surface-enhanced Raman sensing of insulin in the secretions from human pancreatic islets under low and high glucose environments without the use of labels such as antibodies or aptamers. Label-free measurements of the islet secretions showed excellent correlation among the ambient glucose levels, secreted insulin concentrations, and measured Raman-emission intensities. When excited at 785 nm, plasmonic hotspots of the densely arranged 3D gold-nanoparticle pillars as well as strong interaction between sulfide linkages of the insulin molecules and the gold nanoparticles produced highly sensitive and reliable insulin measurements down to 100 pM. The sensors exhibited a dynamic range of 100 pM to 50 nM with an estimated detection limit of 35 pM, which covers the reported concentration range of insulin observed in pancreatic cell secretions. The sensitivity of this approach is approximately 4 orders of magnitude greater than previously reported results using label-free optical approaches, and it is much more cost-effective than immunoassay-based insulin detection widely used in clinics and laboratories. These promising results may open up new opportunities for insulin sensing in research and clinical applications.

Localized Liquid-Phase Synthesis of Porous SnO2 Nanotubes on MEMS Platform for Low-Power, High Performance Gas Sensors.

We have developed highly sensitive, low-power gas sensors through the novel integration method of porous SnO2 nanotubes (NTs) on a micro-electro-mechanical-systems (MEMS) platform. As a template material, ZnO nanowires (NWs) were directly synthesized on beam-shaped, suspended microheaters through an in situ localized hydrothermal reaction induced by local thermal energy around the Joule-heated area. Also, the liquid-phase deposition process enabled the formation of a porous SnO2 thin film on the surface of ZnO NWs and simultaneous etching of the ZnO core, eventually to generate porous SnO2 NTs. Because of the localized synthesis of SnO2 NTs on the suspended microheater, very low power for the gas sensor operation (<6 mW) has been realized. Moreover, the sensing performance (e.g., sensitivity and response time) of synthesized SnO2 NTs was dramatically enhanced compared to that of ZnO NWs. In addition, the sensing performance was further improved by forming SnO2-ZnO hybrid nanostructures due to the heterojunction effect.

Simple, Large-Scale Fabrication of Uniform Raman-Enhancing Substrate with Enhancement Saturation.

It is well-known that gold nanoparticle (AuNP) clusters generate strong surface-enhanced Raman scattering (SERS). In order to produce spatially uniform Raman-enhancing substrates at a large scale, we synthesized vertically perforated three-dimensional (3D) AuNP stacks. The 3D stacks were fabricated by first hydrothermally synthesizing ZnO nanowires perpendicular to silicon wafers followed by repetitively performing liquid-phase deposition of AuNPs on the tops and side surfaces of the nanowires. During the deposition process, the nanowires were shown to gradually dissolve away, leaving hollow vestiges or perforations surrounded by stacks of AuNPs. Simulation studies and experimental measurements reveal these nanoscale perforations serve as light paths that allow the excitation light to excite deeper regions of the 3D stacks for stronger overall Raman emission. Combined with properly sized nanoparticles, this feature maximizes and saturates the Raman enhancement at 1-pM sensitivity across the entire wafer-scale substrate, and the saturation improves the wafer-scale uniformity by a factor of 6 when compared to nanoparticle layers deposited directly on a silicon wafer substrate. Using the 3D-stacked substrates, quantitative sensing of adenine molecules yielded concentrations measurements within 10% of the known value. Understanding the enhancing mechanisms and engineering the 3D stacks have opened a new method of harnessing the intense SERS observed in nanoparticle clusters and realize practical SERS substrates with significantly improved uniformity suitable for quantitative chemical sensing.

Multiplexed gas sensor based on heterogeneous metal oxide nanomaterial array enabled by localized liquid-phase reaction.

A novel method for the selective and localized synthesis of nanomaterials and their in situ integration based on serial combination of localized liquid-phase reaction has been developed for the fabrication of heterogeneous nanomaterial array. This method provides simple, fast and cost-effective fabrication process by using well-controlled thermal energy and therefore solves the challenging problems of assembly and integration of heterogeneous nanomaterial array in functional microelectronic devices. We have fabricated a parallel array of TiO2 nanotubes, CuO nanospikes, and ZnO nanowires, which exhibited adequate gas sensing response. Furthermore, we could approximately determine individual gas concentrations in a mixture gas consisting of 0-2 ppm of NO2 and 0-800 ppm of CO gas species by analyzing multiple data from an array of heterogeneous sensing nanomaterials.

Fabrication of heterogeneous nanomaterial array by programmable heating and chemical supply within microfluidic platform towards multiplexed gas sensing application.

A facile top-down/bottom-up hybrid nanofabrication process based on programmable temperature control and parallel chemical supply within microfluidic platform has been developed for the all liquid-phase synthesis of heterogeneous nanomaterial arrays. The synthesized materials and locations can be controlled by local heating with integrated microheaters and guided liquid chemical flow within microfluidic platform. As proofs-of-concept, we have demonstrated the synthesis of two types of nanomaterial arrays: (i) parallel array of TiO2 nanotubes, CuO nanospikes and ZnO nanowires, and (ii) parallel array of ZnO nanowire/CuO nanospike hybrid nanostructures, CuO nanospikes and ZnO nanowires. The laminar flow with negligible ionic diffusion between different precursor solutions as well as localized heating was verified by numerical calculation and experimental result of nanomaterial array synthesis. The devices made of heterogeneous nanomaterial array were utilized as a multiplexed sensor for toxic gases such as NO2 and CO. This method would be very useful for the facile fabrication of functional nanodevices based on highly integrated arrays of heterogeneous nanomaterials.

Focused energy field method for the localized synthesis and direct integration of 1D nanomaterials on microelectronic devices.

In the focused energy field method, localized heating, and convective mass transfer in a liquid precursor realizes selective synthesis and direct integration of 1D nanomaterials as well as their surface functionalization, all in a low-temperature, liquid environment. This allows facile fabrication of 1D nanomaterial-based nanoelectronic devices.

Highly integrated synthesis of heterogeneous nanostructures on nanowire heater array.

We have proposed a new method for the multiplexed synthesis of heterogeneous nanostructures using a top-down fabricated nanowire heater array. Hydrothermally synthesized nanostructures can be grown only on the heated nanowire through nanoscale temperature control using a Joule heated nanowire. We have demonstrated the selective synthesis of zinc oxide (ZnO) nanowires and copper oxide (CuO) nanostructures, as well as their surface modification with noble metal nanoparticles, using a nanowire heater array. Furthermore, we could fabricate an array of heterogeneous nanostructures via Joule heating of individual nanowire heaters and changing of the precursor solutions in a sequential manner. We have formed a parallel array of palladium (Pd) coated ZnO nanowires and gold (Au) coated ZnO nanowires, as well as a parallel array of ZnO nanowires and CuO nanospikes, in the microscale region by using the developed method.

A stretchable strain sensor based on a metal nanoparticle thin film for human motion detection.

Wearable strain sensors for human motion detection are being highlighted in various fields such as medical, entertainment and sports industry. In this paper, we propose a new type of stretchable strain sensor that can detect both tensile and compressive strains and can be fabricated by a very simple process. A silver nanoparticle (Ag NP) thin film patterned on the polydimethylsiloxane (PDMS) stamp by a single-step direct transfer process is used as the strain sensing material. The working principle is the change in the electrical resistance caused by the opening/closure of micro-cracks under mechanical deformation. The fabricated stretchable strain sensor shows highly sensitive and durable sensing performances in various tensile/compressive strains, long-term cyclic loading and relaxation tests. We demonstrate the applications of our stretchable strain sensors such as flexible pressure sensors and wearable human motion detection devices with high sensitivity, response speed and mechanical robustness.