Selective Determination of Dopamine on a Boron‐Doped Diamond Electrode Modified with Gold Nanoparticle/Polyelectrolyte‐coated Polystyrene Colloids

Negatively charged gold nanoparticles (AuNPs) and a polyelectrolyte (PE) have been assembled alternately on a polystyrene (PS) colloid by a layer‐by‐layer (LBL) self‐assembly technique to form three‐dimensional (Au/PAH)₄/(PSS/PAH)₄ multilayer‐coated PS spheres (Au/PE/PS multilayer spheres). The Au/PE/PS multilayer spheres have been used to modify a boron‐doped diamond (BDD) electrode. Cyclic voltammetry is utilized to investigate the properties of the modified electrode in a 1.0 M KCl solution that contains 5.0 × 10^?3 M K₃Fe(CN)₆, and the result shows a dramatically decreased redox activity compared with the bare BDD electrode. The electrochemical behaviors of dopamine (DA) and ascorbic acid (AA) on the bare and modified BDD electrode are studied. The cyclic voltammetric studies indicate that the negatively charged, three‐dimensional Au/PE/PS multilayer sphere‐modified electrodes show high electrocatalytic activity and promote the oxidation of DA, whereas they inhibit the electrochemical reaction of AA, and can effectively be used to determine DA in the presence of AA with good selectivity. The detection limit of DA is 0.8 × 10^?6 M in a linear range from 5 × 10^?6 to 100 × 10^?6 M in the presence of 1 × 10^?3 M AA.     

Ultrasensitive Detection of a Variety of Analytical Targets Based on a Functionalized Low‐Resistance AuNPs/β‐Ni(OH)2 Nanosheets/Ni Foam Sensing Platform

Simple, low‐cost and yet accurate, sensitive, and quantitative detection of a broad range of analytical targets by means of small footprint sensing devices has the potential to revolutionize medical diagnostics, food safety, and environmental monitoring. This work demonstrates a functional nucleic acids (FNAs) tethered AuNPs/β‐Ni(OH)₂ nanosheets (NS)/Ni foam nanocomposite as a miniaturized electrode. Through the rational design of a low‐barrier ohmic contact of AuNPs to β‐Ni(OH)₂ NS and a target mediated nanochannel electron transfer effect, a variety of analytical targets, ranging from a disease marker (thrombin, 16.3 × 10^?12 m detection limit) to an important biological cofactor (adenosine, 3.2 × 10^?12 m detection limit), and to a toxic metal ion (Hg²⁺, 3.1 × 10^?12 m detection limit), are detected with ultrasensitivity. The presence of target triggers the conformational change of FNAs, introducing strong steric hindrance and electrostatic repulsion to the diffusion of electron indicators toward the electrode surface, ultimately leading to the changes in impedance. A novel equivalent circuit considering the capacitive reactance is proposed to describe the 2D NS‐based impedance DNA bioelectrode. This sensing platform is easily applicable to the detection of many other targets in diverse sample matrices through the use of other suitable FNAs materials.     

Quantum‐Dot‐Tagged Bioresponsive Hydrogel Suspension Array for Multiplex Label‐Free DNA Detection

A novel hydrogel suspension array, which possesses the joint advantages of quantum‐dot‐encoded technology, bioresponsive hydrogels, and photonic crystal sensors with full multiplexing label‐free DNA detection capability is developed. The microcarriers of the suspension array are quantum‐dot‐tagged DNA‐responsive hydrogel photonic beads. In the case of label‐free DNA detection, specific hybridization of target DNA and the crosslinked single‐stranded DNA in the hydrogel grid will cause hydrogel shrinking, which can be detected as a corresponding blue shift in the Bragg diffraction peak position of the beads that can be used for quantitatively estimating the amount of target DNA. The results of the label‐free DNA detection show that the suspension array has high selectivity and sensitivity with a detection limit of 10^?9 M . This method has the potential to provide low cost, miniaturization, and simple and real‐time monitoring of hybridization reaction platforms for detecting genetic variations and sequencing genes.     

Light‐Induced Swelling‐Responsive Conductive,Adhesive, and Stretchable Wireless Film Hydrogel as Electronic Artificial Skin

Light‐induced wireless soft electronic skin hydrogels with excellent mechanical and electronic properties are important for several applications, such as soft robotics and intelligent wearable devices. Precise control of reversible stretchability and capacitive properties depending on intermolecular interaction and surface characteristics remains a challenge. Here, a thin‐film hydrogel is designed based on titanium oxide (TiO₂) polydopamine–perfluorosilica carbon dot‐conjugated chitosan–polyvinyl alcohol‐loaded tannic acid with controllable hydrophobic–hydrophilic transition in the presence of UV–vis light irradiation. The shifting of surface wettability from hydrophobic to hydrophilic by irradiation affects thin‐film water permeability and swelling ratio. This allows the penetration of water into the matrix to change its mechanical strength, electronic properties, and adhesive behavior. Specifically, the hydrogel displays mechanical strain as high as 278% in response to light stimuli and demonstrates the ability to regain its initial state determining the elasticity of the fabricated material. Moreover, the thin‐film hydrogel shows an increase in conductivity to 1.096 × 10^?3 and 1.026 × 10^?3 S cm^?1 when irradiated with UV and visible light, respectively. The hydrogel exhibits capacitive reversibility that follows finger motion which can be identified directly or remotely using wireless connection, indicative of its possible applications as an artificial electronic skin.     

Scissor‐Like Chiral Metamolecules for Probing Intracellular Telomerase Activity

A DNA‐driven gold (Au) heterodimer for intracellular telomerase detection is fabricated. The highly biocompatible and intracellularly stable probe shows an active chiroptical property in the visible region, due to the scissor‐like configuration formed by prolate nanoparticles. Importantly, the telomerase activity is specifically quantified using circular dichroism intensity in situ after internalization of the heterodimer into cancer cells. Moreover, the results clearly illustrate that this method has a remarkable linear range from 0.8 × 10^?12 to 32 × 10^?12 IU, and the limit of detection for telomerase activity is 1.7 × 10^?15 IU in a single HeLa cell. This strategy paves the way for chirality‐based ultrasensitive detection of intracellular cancer markers.     

Synthesis and Characterization of Luminescent Eu(TTA)3phen in a Poly(ethylene oxide) Matrix for Detecting Traces of Water

The water vapor transmission rate (WVTR) is limited to 10^?6 g/m²/day for flexible organic light-emitting diodes. However, it is difficult to measure permeability as low as 10^?6 g/m²/day with current commercial testing methods. To address this need, a developed optochemical method which is extremely sensitive to oxygen or water shows promise. In this study, an Eu complex is synthesized and characterized as a fluorescent probe for detecting traces of water molecules. The Eu-complex film dispersed in poly(ethylene oxide) has strong red fluorescence that is easily quenched by a trace of water. Based on the photoluminescence spectra, the detection limit of the film to water appears to be below 1.0 × 10^?9 g/cc. This suggests that the Eu-complex film can be used as a film sensor to measure WVTRs below 10^?6 g/m²/day.     

A Universal,Label‐Free,and Sensitive Optical Enzyme‐Sensing System for Nuclease and Methyltransferase Activity Based on Light Scattering of Carbon Nanotubes

A label‐free, enzyme‐responsive nanosystem that uses a DNA/single‐walled carbon nanotube (SWNT) assembly as the substrate is demonstrated for the sensitive, universal detection of restriction and nonrestriction endonucleases as well as methyltransferases in a homogeneous solution on the basis of light scattering (LS) of carbon nanotubes. This protocol is based on the different binding affinities of SWNTs to single‐ and double‐stranded DNA. This difference can lead to different LS signals that can be used for the detection of nuclease cleavage activity. The assay only requires a label‐free oligonucleotide probe, significantly reducing the typical cost. The LS technique and the use of a nuclease‐specific oligonucleotide probe impart extraordinarily high sensitivity and selectivity. This light scattering assay is universal and label‐free with a detection limit of 5 × 10^?6 U μL^?1 for S1 nuclease, 1 × 10^?4 U μL^?1 for EcoRI endonuclease, and 1 × 10^?2 U μL^?1 for EcoRI methylase. In principle, this assay can be used to detect any kind of nuclease by simply changing the DNA sequences of the specific probe.     

A Simple and Innovative Route to Prepare a Novel Carbon Nanotube/Prussian Blue Electrode and its Utilization as a Highly Sensitive H2O2 Amperometric Sensor

The utilization of iron‐based species (mainly metallic iron, hematite and magnetite) encapsulated into multi‐walled carbon nanotubes (CNTs) as reactants in an electrochemical synthesis is reported for the first time in this work. Prussian blue (PB) is electrosynthesized in a heterogeneous reaction between ferricyanide ions in aqueous solution and the iron‐species encapsulated into CNTs, resulting in novel CNT/PB paste electrodes. This innovative preparation route produces an intimate contact between the PB and the CNTs, which improves the stability and redox properties of PB. The PB formation and the chemical interaction between the PB and the CNTs are confirmed by Raman spectroscopy. The electrode is employed as a hydrogen peroxide amperometric sensor, resulting in a very low limit of detection (1.94 × 10^?8 mol L^?1) and very high sensitivity (15.3 A cm^?2 M ^?1).     

Nanoscale Graphene Doped with Highly Dispersed Silver Nanoparticles: Quick Synthesis,Facile Fabrication of 3D Membrane‐Modified Electrode,and Super Performance for Electrochemical Sensing

The performance of graphene‐based hybrid materials greatly depends on the dispersibility of nanoscale building blocks on graphene sheets. Here, a quick green synthesis of nanoscale graphene (NG) nanosheets decorated with highly dispersed silver nanoparticles (AgNPs) is demonstrated, and then the electrospinning technique to fabricate a novel nanofibrous membrane electrode material is utilized. With this technique, the structure, mechanical stability, biochemical functionality, and other properties of the fabricated membrane electrode material can be easily controlled. It is found that the orientations of NG and the dispersity of AgNPs on the surface of NG have significant effects on the properties of the fabricated electrode. A highly sensitive H₂O₂ biosensor is thus created based on the as‐prepared polymeric NG/AgNP 3D nanofibrous membrane‐modified electrode (MME). As a result, the fabricated biosensor has a linear detection range from 0.005 to 47 × 10^?3m (R = 0.9991) with a supralow detection limit of 0.56 × 10^?6m (S/N = 3). It is expected that this kind of nanofibrous MME has wider applications for the electrochemical detection and design of 3D functional nanomaterials in the future.     

Desalination by Electrodialysis Using a Stack of Patterned Ion‐Selective Hydrogels on a Microfluidic Device

This study reports a novel approach for separation of charged species using anion‐exchange hydrogel (AEH) and cation‐exchange hydrogel (CEH) in a microfluidic device. The capillary line pinning technique, which is applied in this study, enables in situ fabrication of alternating AEH and CEH that are placed in confined compartments. Adjacent enriched and depleted streams are obtained in continuous flow when a potential difference is applied over the hydrogel stack. The desalination performance of the microchip is demonstrated at different salt concentrations (0.01 × 10^?3–1× 10^?3m sodium chloride), potentials (10–100 V), current densities (12–28 A m^?2), and liquid flow rates (0–5 µL min^?1). It is shown that the microchip is able to remove ≈75% of the salt initially present in the depleted outlet streams at inlet stream concentrations of 1 × 10^?3m sodium chloride. Besides desalination, the microchip allows study of ion transport in the ion‐selective hydrogels to elucidate the interplay of transport phenomena at the electrolyte–hydrogel interface during the desalination process.     

Highly conducting and transparent Ga2O3 doped ZnO thin films prepared by thermal evaporation method

Amorphous zinc oxide thin films are obtained by thermally evaporating pure zinc oxide powder. Films obtained have an excellent conductivity of 90 ??^?1 cm^?1 with transparency of up to 90% in the visible region. On doping with gallium oxide a great improvement in the conductivity of up to 8.7 × 10³ ??^?1 cm^?1 is observed and the optical band gap of the films is decreased from 3.25 to 3.2 eV, retaining the transparency. Measurements of activation energy show that the doped ZnO film has one donor level at 68 meV and other at 26 meV bellow the conduction band.     

Enhanced Performance of GaN-Based Green Light-Emitting Diodes with Gallium-Doped ZnO Transparent Conducting Oxide

Ga-doped ZnO (GZO) transparent conducting oxide was grown by oxygen plasma-enhanced pulsed laser deposition. GZO grown in the presence of oxygen radicals had resistivity of 1 × 10^?3 Ω cm and average visible (500–700 nm) transmittance of 92.5%. A low specific contact resistance of 6.5 × 10^?4 Ω cm² of GZO on p-GaN was achieved by excimer laser annealing (ELA) treatment of p-GaN before GZO electrode deposition. The ELA-treated light emitting diode (LED) fabricated with the GZO electrode as a current-spreading layer resulted in light-output power enhanced by 56.2% at 100 mA compared with that fabricated with a conventional Ni/Au metal electrode. The high-light output and low degradation of light-output power were attributed to the decrease in contact resistance between the p-GaN layer and the GZO electrode and uniform current spreading over the p-GaN layer. In addition, low contact resistance results in a decrease of self-heat generation during current drive.     

Metallic conductivity over an acceptor band of lightly compensated copper-doped p-Hg0.78Cd0.22Te crystals

The conductivity and Hall effect of heavily doped p-Hg_0.78Cd_0.22Te:Cu crystals were studied in the temperature range of 4.2–125 K. The conductivity over the impurity band is of a metallic type for the acceptor concentration N _A>3.8×10¹⁷ cm^?3. The conductivity and the Hall coefficient governed by the delocalized charge carriers in the impurity band are independent of temperature. The sign of the Hall effect is positive in the metallic conductivity range. Near the metal-insulator transition point, the Hall mobility increases linearly with the acceptor concentration and is independent of the acceptor concentration at N _A>1.6×10¹⁸ cm^?3. The metallic conductivity is proportional to N _A in the concentration range under study at N _A<3.1×10¹⁸ cm^?3. The Anderson transition occurs at the Cu concentration N _A=1.4×10¹⁷ cm^?3 in the A ⁺ impurity band, which is formed by positively charged acceptors. Minimum metallic conductivity corresponding to this transition equals 5.1 Ω^?1 cm^?1. It is shown that ?₂ conductivity in the subthreshold region is defined by delocalized carriers in the upper Hubbard band only for fairly heavy doping (N _A>1.4×10¹⁷ cm^?3). For N _A<1.4×10¹⁷ cm^?3, the hopping conductivity is observed.     

Gold‐Cluster Sensors Formed Electrochemically at Boron‐Doped‐Diamond Electrodes: Detection of Dopamine in the Presence of Ascorbic Acid and Thiols

Gold clusters have been electrodeposited on a boron‐doped diamond (BDD) electrode by scanning the potential from 0.7 V to 0.0 V (vs. 3 M KCl‐Ag/AgCl reference) in a solution of 0.5 mM KAuCl₄ and 1.0 M KCl. The cluster‐modified diamond (Au/BDD) electrode has been used to investigate the oxidative properties of dopamine (DA) and ascorbate (AA). The modified diamond electrode shows a higher activity for DA oxidation than AA; the oxidation potential of DA shifted to a less‐positive potential (0.11 V) than that of AA, which oxidized at 0.26 V, and DA possesses a much higher peak current than that of AA. The reversibility of the electrode reaction with DA is significantly improved at the Au/BDD electrode, which results in a large increase in the square‐wave voltammetric peak current, with a detection limit of 0.1 μM in the presence of a large excess of AA. The Au/BDD electrode shows excellent sensitivity and good selectivity for DA detection. A self‐assembled monolayer (SAM) of mercaptoacetic acid on the Au clusters was used to provide an antifouling effect as the negative CO₂^– groups repulse negative ascorbate and attract positive dopamine in pH 7.4 buffer. After pre‐absorption, the SAM/Au/BDD electrode could detect 1.0 nM DA in a linear range from 10 nM to 10 μM in the presence of 10^–4 M AA.     

Electrical properties of ultrathin oxide grown by high pressure oxidation and N2O nitridation for ULSI device applications

For the first time, the feasibility of ultrathin oxides grown by high pressure oxidation (HIPOX) technology in O₂ ambient and nitrided in N₂O ambient with rapid thermal processing has been investigated in order for them to be used as a gate oxide of ULSI devices. The dielectric breakdown electric field (E _BR) and the midgap interface trap density (D _itm) of the nitrided-HIPOX oxide are ?13:9MVcm^?1 and 2 × 10¹⁰cm^?2eV^?1 respectively which are almost the same as those of the control oxide and the nitrided-control oxide. The time-tobreakdown (t_BD) of the nitrided-HIPOX oxide is longer than that of the control oxide at low electric field (<10^?4 A cm^?2) owing to the combination of nitrogen and defects near the Si?SiO₂ interface during nitridation. The lifetimes of the nitrided-HIPOX oxides increase initially, reaching a maximum value of 1:2 × 10⁹ s at a stress current density of 1 × 10^?6 A cm^?2,corresponding to over 10 years, and then decrease as nitridation proceeds.     

Novel iron (III) phthalocyanine derivative functionalized semiconductor based transducers for the detection of citrate

In the present work, we report a novel citrate-selective sensor based on iron (III) phthalocyanine chloride-C-monoamido-Poly-n-Butyl Acrylate (Fe(III)MAPcCl-P-n-BA) modified silicon nitride and Ion sensitive field effect transistor (ISFET) structures for the electrochemical determination and estimation of the pathophysiological range of citrate. The developed capacitive sensor based on Fe(III)MAPcCl-P-n-BA had a Nernstian sensitivity of (−20.2 ± 1.3) mV/decade with a detection limit of about 7 × 10⁻⁷ M and a linear range from 10⁻⁶ M to 10⁻¹ M (RSD = 6.2%). Then, the performance of the Fe(III)MAPcCl-P-n-BA functionalized ISFET structure towards the detection of citrate has been investigated. A Nernstian sensitivity of about (−19.8 ± 1.0) mV/decade in the range from 10⁻⁶ M to 10⁻¹ M was achieved (RSD = 4.8%) which covered the pathologically important clinical range of citrate. The detection limit was about 4 × 10⁻⁷ M. The number of available recognition sites N_s and the complexation constant pK were calculated using the enhanced site binding model. A side by side comparison of the developed chemical sensors based on electrolyte-insulator-Semi conductor (EIS) and ISFET structures showed similar characteristics which proves the successful miniaturization of the semiconductor based transducer. The obtained experimental data of the Fe(III)MAPcCl-P-n-BA functionalized ISFET structure were used to validate the TopSPICE ISFET/MEMFET macromodel. The obtained theoretical sensitivity was in good agreement to the experimental one which proves the successful design of the developed ISFET/MEMFET macromodel.     

Current-voltage characteristics of electric contacts on p-type ZnSe

The current-voltage characteristics of electric contacts made of different materials on p-type ZnSe that form Schottky barriers from 0.3 to 1.2 eV are studied theoretically using the formula $$J = \frac{{A^* T}}{k}\int_0^\infty {T(E)[F(E) - F(E - eV)]dE,} $$ where T(E) is the energy-dependent quantum tunneling probability and F(E) is the Fermi distribution function. The contribution to the total current of both the thermionic emission and the tunneling are therefore included. The net doping concentrations under study range from 1.0×10¹⁷ cm^?3 to 1.0×10¹⁹ cm^?3. The reverse bias voltage across the barrier at a current density of 200 A/cm² is used to assess whether the barrier is reduced to an ohmic contact. A barrier of 0.3 eV is already an ohmic contact at doping concentration p=1.0×10¹⁷ cm^?3, while a barrier of 1.2 eV still behaves like a diode event at p=1.0×10¹⁹ cm^?3.     

Scattering of phonons by a spatially correlated system of Fe atoms and the low-temperature anomaly of thermal conductivity in HgSe:Fe crystals

The thermal conductivity κ of HgSe:Fe samples with various content N _Fe of Fe impurity was studied in the temperature range of 8–60 K. It was found that the dependence of the thermal conductivity κ on N _Fe is unconventional at low temperatures. For T<12 K, the value of κ first decreases with an increase in the Fe concentration up to N _Fe=5×10¹⁸ cm^?3 and then increases and attains a maximum for N _Fe=(1–2)×10¹⁹ cm^?3. A further increase in Fe concentration brings about a steady decrease in thermal conductivity. The electron-and phonon-related thermal conductivity of HgSe:Fe crystals with consideration of the effects caused by the ordering of trivalent Fe ions was analyzed. It is shown that both the electron-and phonon-related contributions to thermal conductivity at low temperatures are increasing functions of Fe concentration in the range of 5×10¹⁸<N _Fe<(1–2)×10¹⁹ cm^?3. However, the electronic contribution is too small to account for the experimental increase in thermal conductivity. An analysis of the lattice contribution to thermal conductivity showed that an anomalous increase in thermal conductivity is caused by a reduction in the Rayleigh scattering of phonons by a system of Fe ions with mixed valence and is related to the spatial ordering of Fe³⁺ ions.     

Large‐Area Silver‐Coated Silicon Nanowire Arrays for Molecular Sensing Using Surface‐Enhanced Raman Spectroscopy

A new and facile method to prepare large‐area silver‐coated silicon nanowire arrays for surface‐enhanced Raman spectroscopy (SERS)‐based sensing is introduced. High‐quality silicon nanowire arrays are prepared by a chemical etching method and used as a template for the generation of SERS‐active silver‐coated silicon nanowire arrays. The morphologies of the silicon nanowire arrays and the type of silver‐plating solution are two key factors determining the magnitude of SERS signal enhancement and the sensitivity of detection; they are investigated in detail for the purpose of optimization. The optimized silver‐coated silicon nanowire arrays exhibit great potential for ultrasensitive molecular sensing in terms of high SERS signal enhancement ability, good stability, and reproducibility. Their further applications in rapidly detecting molecules relating to human health and safety are discussed. A 10 s data acquisition time is capable of achieving a limit of detection of approximately 4 × 10^?6 M calcium dipicolinate (CaDPA), a biomarker for anthrax. This value is 1/15 the infectious dose of spores (6 × 10^?5 M required), revealing that the optimized silver‐coated silicon nanowire arrays as SERS‐based ultrasensitive sensors are extremely suitable for detecting Bacillus anthracis spores.     

Highly transparent and conducting zinc oxide films deposited by activated reactive evaporation

Highly transparent and conducting undoped zinc oxide films have been obtained with a best resistivity of ～1.1 × 10^-3 Ω cm, a carrier density of ～1.5 × 10²⁰ cm^?3 and a mobility of ～38 cm²V^{?1s ?1}. These were produced by activated reactive evaporation at a deposition rate of 2 to 8Å/s with a substrate temperature ≤200° C. The films deposited by this process were found to have resistivities that were thickness independent and also were relatively insensitive to deposition parameters. In terms of conductivity, it was found that films deposited at higher temperatures (T > 300°+ C) were always inferior to the films deposited below 200° C. High temperature vacuum annealing (350° C) significantly degraded the resistivity of the undoped films deposited at low temperature; this was attributable to a drop in both the electron concentration and the mobility. Aluminum doping was found to be able to stabilize the electron concentration while the drop in mobility was found to be related to the choice of substrate.