Carbon Nanosheets Infused with Gold Nanoparticles as an Ultrasensitive Nose for Electrochemical Arsenic Sensing.

Herein, we introduce an eco-friendly electrochemical sensor based on melamine-enriched nitrogen-doped carbon nanosheets decorated with gold nanoparticles (Au-CNSm) for arsenic sensing. An extremely facile, low-toxicity, biocompatible, and affordable hydrothermal technique was adopted for the synthesis of the Au-CNSm nanocomposite. The Au-CNSm-integrated sensing platform was optimized for electrode composition by cyclic voltammetry (CV). Owing to the synergistic effects of melamine-enriched carbon nanosheets (CNSm) and gold nanoparticles (AuNPs), the anodic peak current increased in the Au-CNSm-modified sensing electrode as compared to the CNSm-decorated platform. A wide linear range of 0.0001-100 µM and a low detection limit of 0.0001 µM were obtained. The visual signals can be measured at a very minute concentration of 0.0001 µM (0.1 ppb) on a screen-printed carbon electrode (SPCE) modified with Au-CNSm. Hence, this electrode system clearly outperformed the previously reported studies in terms of linear range, limit of detection (LOD), and electrocatalytic activity for arsenic sensing. Interestingly, the fabricated biosensor can be developed as a point-of-care device for real-time environmental monitoring for public safety. Henceforth, owing to exceptional attributes such as portability, selectivity, and sensitivity, this device offers great promise in modeling a revolutionary new class of electrochemical sensing platforms for an ultrasensitive and reliable detection strategy for arsenite (As(III)).

Resistive switching and battery-like characteristics in highly transparent Ta2O5/ITO thin-films.

Highly transparent resistive-switching (RS) devices were fabricated by growing amorphous tantalum pentoxide (a-Ta2O5) and indium tin oxide (a-ITO) thin films on barium-borosilicate glass (7059) substrates, using electron beam evaporation. These layers exhibited the transmittance greater than ~ 85% in the full visible region and showed RS behavior and battery-like IV characteristics. The overall characteristics of RS can be tuned using the top electrode and the thickness of a-Ta2O5. Thinner films showed a conventional RS behavior, while thicker films with metal electrodes showed a battery-like characteristic, which could be explained by additional redox reactions and non-Faradaic capacitive effects. Devices having battery-like IV characteristics showed higher enhanced, retention and low-operation current.

Unravelling oxygen driven α to ß phase transformation in tungsten.

Thin films of ß-W are the most interesting for manipulating magnetic moments using spin-orbit torques, and a clear understanding of α to ß phase transition in W by doping impurity, especially oxygen, is needed. Here we present a combined experimental and theoretical study using grazing incidence X-ray diffraction, photoelectron spectroscopy, electron microscopy, and ab initio calculations to explore atomic structure, bonding, and oxygen content for understanding the formation of ß-W. It is found that the W films on SiO2/Si have 13-22 at.% oxygen in A15 ß structure. Ab initio calculations show higher solution energy of oxygen in ß-W, and a tendency to transform locally from α to ß phase with increasing oxygen concentration. X-ray absorption spectroscopy also revealed local geometry of oxygen in ß-W, in agreement with the simulated one. These results offer an opportunity for a fundamental understanding of the structural transition in α-W and further development of ß-W phase for device applications.

Spontaneous Reduction of Copper(II) to Copper(I) at Solid-Liquid Interface.

Oxidation and reduction reactions are of central importance in chemistry as well as vital to the basic functions of life and such chemical processes are generally brought about by oxidizing and reducing agents, respectively. Herein, we report the discovery of an interfacial reduction reaction (IRR) - without the use of any external reducing agent. In course of metal-ligand coordination, spontaneous reduction of Cu(II) to Cu(I) at a solid-liquid interface was observed-unlike in a liquid-phase reaction where no reduction of Cu(II) to Cu(I) was occurred. High-quality thin films of a new coordination network compound bearing a Fe(II)-CN-Cu(I) link were fabricated by IRR and employed for efficient electro-catalysis in the form of oxygen reduction reaction. Also, thermally activated reversible structural phase transition modulated the electron transport property in thin film. This work unveils the importance of chemical reactions at solid-liquid interfaces that can lead to the development of new functional thin film materials.

Layer-by-Layer-Assembled AuNPs-Decorated First-Generation Poly(amidoamine) Dendrimer with Reduced Graphene Oxide Core as Highly Sensitive Biosensing Platform with Controllable 3D Nanoarchitecture for Rapid Voltammetric Analysis of Ultratrace DNA Hybridization.

The structure and electrochemical properties of layer-by-layer-assembled gold nanoparticles (AuNPs)-decorated first-generation (G1) poly(amidoamine) dendrimer (PD) with reduced graphene oxide (rGO) core as a highly sensitive and label-free biosensing platform with a controllable three-dimensional (3D) nanoarchitecture for the rapid voltammetric analysis of DNA hybridization at ultratrace levels were characterized. Mercaptopropinoic acid (MPA) was self-assembled onto Au substrate, then GG1PD formed by the covalent functionalization between the amino terminals of G1PD and carboxyl terminals of rGO was covalently linked onto MPA, and finally AuNPs were decorated onto GG1PD by strong physicochemical interaction between AuNPs and -OH of rGO in GG1PD, which was characterized through different techniques and confirmed by computational calculation. This 3D controllable thin-film electrode was optimized and evaluated using [Fe(CN)6]3-/4- as the redox probe and employed to covalently immobilize thiol-functionalized single-stranded DNA as biorecognition element to form the DNA nanobiosensor, which achieved fast, ultrasensitive, and high-selective differential pulse voltammetric analysis of DNA hybridization in a linear range from 1 × 10-6 to 1 × 10-13 g m-1 with a low detection limit of 9.07 × 10-14 g m-1. This work will open a new pathway for the controllable 3D nanoarchitecture of the layer-by-layer-assembled metal nanoparticles-functionalized lower-generation PD with two-dimensional layered nanomaterials as cores that can be employed as ultrasensitive and label-free nanobiodevices for the fast diagnosis of specific genome diseases in the field of biomedicine.

Intermediate stages of surface state formation and collapse of topological protection to transport in Bi2Se3.

Surface states consisting of helical Dirac fermions have been extensively studied in three-dimensional topological insulators. Yet, experiments to date have only investigated fully formed topological surface states (TSS) and it is not known whether preformed or partially formed surface states can exist or what properties they could potentially host. Here, by decorating thin films of Bi2Se3 with nanosized islands of the same material, we show for the first time that not only can surface states exist in various intermediate stages of formation but they exhibit unique properties not accessible in fully formed TSS. These include tunability of the Dirac cone mass, vertical migration of the surface state wave-function and the appearance of mid-gap Rashba-like states as exemplified by our theoretical model for decorated TIs. Our experiments show that an interplay of Rashba and Dirac fermions on the surface leads to an intriguing multi-channel weak anti-localization effect concomitant with an unprecedented tuning of the topological protection to transport. Our work offers a new route to engineer topological surface states involving Dirac-Rashba coupling by nano-scale decoration of TI thin films, at the same time shedding light on the real-space mechanism of surface state formation in general.

Magnetic properties and electronic structure of Mn-Ni-Ga magnetic shape memory alloys.

Influence of disorder, antisite defects, martensite transition and compositional variation on the magnetic properties and electronic structure of Mn(2)NiGa and Mn(1+x)Ni(2-x)Ga magnetic shape memory alloys have been studied by using full potential spin-polarized scalar relativistic Korringa-Kohn-Rostocker (FP-SPRKKR) method. Mn(2)NiGa is ferrimagnetic and its total spin moment increases when disorder in the occupancy of MnNi (Mn atom in Ni position) is considered. The moment further increases when Mn-Ga antisite defect [1] is included in the calculation. A reasonable estimate of TC for Mn(2)NiGa is obtained from the exchange parameters for the disordered structure. Disorder influences the electronic structure of Mn(2)NiGa through overall broadening of the density of states and a decrease in the exchange splitting. Inclusion of antisite defects marginally broaden the minority spin partial DOS (PDOS), while the majority spin PDOS is hardly affected. For Mn(1+x)Ni(2-x)Ga where 1 ⩾ x ⩾ 0, as x decreases, Mn(Mn) moment increases while Mn(Ni) moment decreases in both austenite and martensite phases. For x ⩾ 0.25, the total moment of the martensite phase is smaller compared to the austenite phase, which indicates possible occurrence of inverse magnetocaloric effect. We find that the redistribution of Ni 3d- Mn(Ni) 3d minority spin electron states close to the Fermi level is primarily responsible for the stability of the martensite phase in Mn-Ni-Ga.

Influence of the contact potential and space-charge effect on the performance of a Stoffel-Johnson design electron source for inverse photoemission spectroscopy.

By imaging the spatial intensity distribution of the electrons from a Stoffel-Johnson (SJ) type low energy electron source for inverse photoemission spectroscopy (IPES), we find that the focus is distorted when the beam current exceeds the limiting value due to space charge effect. The space charge effect and the contact potential difference suppress the beam current at low energies (<10 eV). In this work, we show that these limitations of the SJ source can be overcome by compensation of the contact potential difference between the cathode and the lens electrodes and an uniform well focused electron beam with the set kinetic energy can be obtained. The size of the electron beam is around 1 mm full width at half maximum over the whole energy range of 5 to 30 eV generally used for IPES. The compensation of the contact potential difference also enhances the beam current substantially at low energies (<10 eV) and uniform beam current is achieved for the whole energy range. We find that the drift in the electron beam position is sensitive to the lens electrode separation and it is about 1 mm over the whole energy range. By measuring the n = 1 image potential state on Cu(100), we show that the resolution is better when the cathode filament current is set to lower values.