Charge-Gradient-Induced Ferroelectricity with Robust Polarization Reversal.

Developing a ferroelectric tunnel junction with a robust polarization reversal is essential for errorless data storage, but it remains challenging since the second-order phase transition dominates the reversal and introduces intermediate states. This investigation has proposed a charge-gradient-induced ferroelectricity, which is featured with the first-order phase transition. As an order parameter, a charge-gradient-induced polarization is achieved by modulation of stoichiometric oxygen along the Bi2O2Se/Bi2Se3O9 bilayer during pulsed laser deposition. At room temperature, this polarity points out-of-plane and shows an abrupt reversal in the ferroelectric hysteresis loop. The coercive field only increases by 0.04 V/nm after 300 reversals. Fabricated into the ferroelectric tunnel junction, the bilayer ferroelectric exhibits a comparable electroresistance of 100. The ON/OFF state can be switched repeatedly or after a 360 s retention. Characterizations of scanning capacitance microscopy and the current-voltage relation demonstrate that the ON/OFF switching is based on an injection exchange between the tunnelling and the thermionic emission.

Exploitation of Schottky-Junction-based Sensors for Specifically Detecting ppt-Concentration Gases.

Gas species and concentrations of human-exhaled breath correlate with health, wherein disease markers contain volatile organic compounds (VOCs) of concentrations in parts per billion. It is expected that a gas-sensing strategy possesses a gas specificity and detection limit in the parts per trillion (ppt) range; however, it is still a challenge. This investigation has exploited the Schottky junction of gas sensors for detecting the reactance signal of ppt VOC, aiming for a specific and rapid detection toward disease marker acetone. In this new sensing paradigm, formed by the engineered energy band between metal-semiconductor contact, the Schottky junction is accessed to specific modulation of different adsorbate dopings and the corresponding reactance signal is measured. Regarding the detection toward ppt concentration of acetone, this sensing paradigm possesses rapid (∼100 s) and room-temperature response, molecular specificity, and 34 ppt of detection limit. The proposed detection paradigm is demonstrated to show a high feasibility toward detection of disease marker acetone.

Research and Verification of Convolutional Neural Network Lightweight in BCI.

With the increasing of depth and complexity of the convolutional neural network, parameter dimensionality and volume of computing have greatly restricted its applications. Based on the SqueezeNet network structure, this study introduces a block convolution and uses channel shuffle between blocks to alleviate the information jam. The method is aimed at reducing the dimensionality of parameters of in an original network structure and improving the efficiency of network operation. The verification performance of the ORL dataset shows that the classification accuracy and convergence efficiency are not reduced or even slightly improved when the network parameters are reduced, which supports the validity of block convolution in structure lightweight. Moreover, using a classic CIFAR-10 dataset, this network decreases parameter dimensionality while accelerating computational processing, with excellent convergence stability and efficiency when the network accuracy is only reduced by 1.3%.

Exploiting Two-Dimensional Bi2 O2 Se for Trace Oxygen Detection.

We exploit a high-performing resistive-type trace oxygen sensor based on 2D high-mobility semiconducting Bi2 O2 Se nanoplates. Scanning tunneling microscopy combined with first-principle calculations confirms an amorphous Se atomic layer formed on the surface of 2D Bi2 O2 Se exposed to oxygen, which contributes to larger specific surface area and abundant active adsorption sites. Such 2D Bi2 O2 Se oxygen sensors have remarkable oxygen-adsorption induced variations of carrier density/mobility, and exhibit an ultrahigh sensitivity featuring minimum detection limit of 0.25 ppm, long-term stability, high durativity, and wide-range response to concentration up to 400 ppm at room temperature. 2D Bi2 O2 Se arrayed sensors integrated in parallel form are found to possess an oxygen detection minimum of sub-0.25 ppm ascribed to an enhanced signal-to-noise ratio. These advanced sensor characteristics involving ease integration show 2D Bi2 O2 Se is an ideal candidate for trace oxygen detection.

Quantitative Analyses of the Interfacial Properties of Current Collectors at the Mesoscopic Level in Lithium Ion Batteries by Using Hierarchical Graphene.

At the mesoscopic level of commercial lithium ion battery (LIB), it is widely believed that the poor contacts between current collector (CC) and electrode materials (EM) lead to weak adhesions and large interfacial electric resistances. However, systematic quantitative analyses of the influence of the interfacial properties of CC are still scarce. Here, we built a model interface between CC and electrode materials by directly growing hierarchical graphene films on commercial Al foil CC, and we performed systematic quantitative studies of the interfacial properties therein. Our results show that the interfacial electric resistance dominates, i.e. ∼2 orders of magnitude higher than that of electrode materials. The interfacial resistance could be eliminated by hierarchical graphene interlayer. Cathode on CC with eliminated interfacial resistance could deliver much improved power density outputs. Our work quantifies the mesoscopic factors influencing the battery performance and offers practical guidelines of boosting the performance of LIBs and beyond.

Robust ultraclean atomically thin membranes for atomic-resolution electron microscopy.

The fast development of high-resolution electron microscopy (EM) demands a background-noise-free substrate to support the specimens, where atomically thin graphene membranes can serve as an ideal candidate. Yet the preparation of robust and ultraclean graphene EM grids remains challenging. Here we present a polymer- and transfer-free direct-etching method for batch fabrication of robust ultraclean graphene grids through membrane tension modulation. Loading samples on such graphene grids enables the detection of single metal atoms and atomic-resolution imaging of the iron core of ferritin molecules at both room- and cryo-temperature. The same kind of hydrophilic graphene grid allows the formation of ultrathin vitrified ice layer embedded most protein particles at the graphene-water interface, which facilitates cryo-EM 3D reconstruction of archaea 20S proteasomes at a record high resolution of ~2.36 Å. Our results demonstrate the significant improvements in image quality using the graphene grids and expand the scope of EM imaging.

Molecular Beam Epitaxy and Electronic Structure of Atomically Thin Oxyselenide Films.

Atomically thin oxychalcogenides have been attracting intensive attention for their fascinating fundamental properties and application prospects. Bi2 O2 Se, a representative of layered oxychalcogenides, has emerged as an air-stable high-mobility 2D semiconductor that holds great promise for next-generation electronics. The preparation and device fabrication of high-quality Bi2 O2 Se crystals down to a few atomic layers remains a great challenge at present. Here, molecular beam epitaxy (MBE) of atomically thin Bi2 O2 Se films down to monolayer on SrTiO3 (001) substrate is achieved by co-evaporating Bi and Se precursors in oxygen atmosphere. The interfacial atomic arrangements of MBE-grown Bi2 O2 Se/SrTiO3 are unambiguously revealed, showing an atomically sharp interface and atom-to-atom alignment. Importantly, the electronic band structures of one-unit-cell (1-UC) thick Bi2 O2 Se films are observed by angle-resolved photoemission spectroscopy (ARPES), showing low effective mass of ≈0.15 m0 and bandgap of ≈0.8 eV. These results may be constructive to the synthesis of other 2D oxychalcogenides and investigation of novel physical properties.

Sensitive Gas-Sensing by Creating Adsorption Active Sites: Coating an SnO2 Layer on Triangle Arrays.

It is a widely used strategy to enhance gas sensor sensitivity by improving its surface area, but this process, including bonding the sensing block into a device substrate, needs complex manipulations. This work shows a concept of creating adsorption active sites, in which an SnO2 layer (6.85 nm thin) is directly coated on a triangle array substrate to be of an ensemble of triangular convex adsorption active sites (TCAASs). The resultant SnO2 gas sensors, with TCAAS periods ranging from 289 to 1154 nm, exhibit an adsorption-active-site-dependent sensitivity and present a low detection limit of around 6 ppm ethanol gas at room temperature. By characterizations of Kelvin force microscopy, a large surface potential variation exists on these adsorption active sites after introducing ethanol gas, distinctly showing a local adsorption enhancement. These results confirm that the creation of adsorption active sites can efficiently increase surface adsorption of a sensor to realize its sensitive gas-sensing.

Carrier Mobility-Dominated Gas Sensing: A Room-Temperature Gas-Sensing Mode for SnO2 Nanorod Array Sensors.

Adsorption-induced change of carrier density is presently dominating inorganic semiconductor gas sensing, which is usually operated at a high temperature. Besides carrier density, other carrier characteristics might also play a critical role in gas sensing. Here, we show that carrier mobility can be an efficient parameter to dominate gas sensing, by which room-temperature gas sensing of inorganic semiconductors is realized via a carrier mobility-dominated gas-sensing (CMDGS) mode. To demonstrate CMDGS, we design and prepare a gas sensor based on a regular array of SnO2 nanorods on a bottom film. It is found that the key for determining the gas-sensing mode is adjusting the length of the arrayed nanorods. With the change in the nanorod length from 340 to 40 nm, the gas-sensing behavior changes from the conventional carrier-density mode to a complete carrier-mobility mode. Moreover, compared to the carrier density-dominating gas sensing, the proposed CMDGS mode enhances the sensor sensitivity. CMDGS proves to be an emerging gas-sensing mode for designing inorganic semiconductor gas sensors with high performances at room temperature.

Template-Assisted Fabrication of Nanostructured Arrays for Sensing Applications.

High sensitivity imposes strict requirements on a sensing platform, for which nanostructured arrays are promising candidates. The template-assisted method is an effective strategy to prepare various nanostructured arrays, which are widely developed for different sensing applications. Herein, nanostructured array based sensing platforms prepared from four widely used templates, a colloidal monolayer, anodic aluminum oxide, block copolymer, and a nanoimprint mold, are reviewed. In a series of sensing applications (e.g., biosensing and gas sensing), the resulting nanostructure-array-based platforms are high sensitive owing to their advanced morphology features: 1) high-density alignment of arrayed nanostructures, 2) high surface-to-volume ratio, and 3) convex-rich morphology. In surface-enhanced Raman spectroscopy (SERS) applications, noble-metal particle arrays with high-density alignment produce an enhanced SERS signal owing to a strong concentration of plasmonic resonance on the substrate. To sense biomolecules in solution and gaseous molecules, arrays with a high surface-to-volume ratio or convex-rich morphology can sensitively respond to changes in the environment. Moreover, the nanostructure-array-based sensing platforms are divided into three types (0D, 1D, and 3D nanostructured arrays) to demonstrate the morphological origin of the sensing performances.

Three-Dimensional Plasmonic Nanostructure Design for Boosting Photoelectrochemical Activity.

Plasmonic nanostructures have been widely incorporated into different semiconductor materials to improve solar energy conversion. An important point is how to manipulate the incident light so that more light can be efficiently scattered and absorbed within the semiconductors. Here, by using a tunable three-dimensional Au pillar/truncated-pyramid (PTP) array as a plasmonic coupler, a superior optical absorption of about 95% within a wide wavelength range is demonstrated from an assembled CdS/Au PTP photoanode. Based on incident photon to current efficiency measurements and the corresponding finite difference time domain simulations, it is concluded that the enhancement is mainly attributed to an appropriate spectral complementation between surface plasmon resonance modes and photonic modes in the Au PTP structure over the operational spectrum. Because both of them are wavelength-dependent, the Au PTP profile and CdS thickness are further adjusted to take full advantage of the complementary effect, and subsequently, an angle-independent photocurrent with an enhancement of about 400% was obtained. The designed plasmonic PTP nanostructure of Au is highly robust, and it could be easily extended to other plasmonic metals equipped with semiconductor thin films for photovoltaic and photoelectrochemical cells.

Reduced Graphene Oxide-Based Ordered Macroporous Films on a Curved Surface: General Fabrication and Application in Gas Sensors.

A new general method for the fabrication of a reduced graphene oxide (rGO)-based ordered monolayer macroporous film composed of a layer of closely arranged pores is introduced. Assisted by the polystyrene microsphere monolayer colloid crystal by a simple solution-heated method, pure rGO, rGO-SnO2, rGO-Fe2O3, and rGO-NiO composite monolayer ordered porous films were examplarily constructed on the curved surface of a ceramic tube widely used in gas sensors. The rGO-oxide composite porous films could exhibit much better sensing performances than those of the corresponding pure oxide films and the composite films without the ordered porous structures in detecting ethanol gas. The enhancement mechanisms induced by distinctive rGO-oxide heterojunctions and porous structures as well as the effects of the rGO content and the pore-size on the sensitivity of the composite films were systematically analyzed and discussed. This study opens up a kind of construction method for an rGO-based composite film gas sensor with uniform surface structures and high performance.

Fabrication of SnO2-reduced graphite oxide monolayer-ordered porous film gas sensor with tunable sensitivity through ultra-violet light irradiation.

A new graphene-based composite structure, monolayer-ordered macroporous film composed of a layer of orderly arranged macropores, was reported. As an example, SnO2-reduced graphite oxide monolayer-ordered macroporous film was fabricated on a ceramic tube substrate under the irradiation of ultra-violet light (UV), by taking the latex microsphere two-dimensional colloid crystal as a template. Graphite oxide sheets dispersed in SnSO4 aqueous solution exhibited excellent affinity with template microspheres and were in situ incorporated into the pore walls during UV-induced growth of SnO2. The growing and the as-formed SnO2, just like other photocatalytic semiconductor, could be excited to produce electrons and holes under UV irradiation. Electrons reduced GO and holes adsorbed corresponding negative ions, which changed the properties of the composite film. This film was directly used as gas-sensor and was able to display high sensitivity in detecting ethanol gas. More interestingly, on the basis of SnO2-induced photochemical behaviours, this sensor demonstrated tunable sensitivity when UV irradiation time was controlled during the fabrication process and post in water, respectively. This study provides efficient ways of conducting the in situ fabrication of a semiconductor-reduced graphite oxide film device with uniform surface structure and controllable properties.

Photochemistry-based method for the fabrication of SnO(2) monolayer ordered porous films with size-tunable surface pores for direct application in resistive-type gas sensor.

A new photochemistry-based method was introduced for fabricating SnO2 monolayer ordered porous films with size-tunable surface pores on ceramic tubes used for gas sensors. The growth of the spherical pore walls was controlled by two times irradiation of the ultraviolet light using polystyrene microsphere two-dimensional colloidal crystal as a template. The surface pore size of the final obtained porous films was well tuned by changing the second irradiation time rather than replacing the template microspheres. The monolayer ordered porous films on the tubes were directly used, for the first time, as gas sensors. The sensitivity of the sensor depended on the surface pore size and was carefully analyzed by ethanol gas detection. The sensor also exhibited short response-recovery time and long-term stability at lower than 300 °C in practical applications. Therefore, this study opens up a kind of construction method for gas sensors, provides a new strategy for controlling the surface pore size of the monolayer ordered porous film, and introduces a new type of sensitivity-controllable gas sensor.