Broadening spectral responses and achieving environmental stability in SnS2/Ag-NPs/HfO2 flexible phototransistors.

Layered two-dimensional (2D) materials have gained popularity thanks to their atomically thin physique and strong coupling with light. Here, we investigated a wide band gap (≥ 2 eV) 2D material, i.e., tin disulfide (SnS2), and decorated it with silver nanoparticles, Ag-NPs, for broadband photodetection. Our results show that the SnS2/Ag-NPs devices exhibit broadband photodetection ranging from the ultraviolet to near-infrared (250-1050 nm) spectrum with decreased rise/decay times from 8/20 s to 7/16 s under 250 nm wavelength light compared to the bare SnS2 device. This is attributed to the localized surface plasmon resonance effect and the wide band gap of SnS2 crystal. Furthermore, the HfO2-passivated SnS2/Ag-NPs devices exhibited high photodetection performance in terms of photoresponsivity (∼12 500 A W-1), and external quantum efficiency (∼6 × 106%), which are significantly higher compared to those of bare SnS2. Importantly, after HfO2 passivation, the SnS2/Ag-NPs photodetector maintained the stable performance for several weeks with merely ∼5.7% reduction in photoresponsivity. Lastly, we fabricated a flexible SnS2/Ag-NPs photodetector, which shows excellent and stable performance under various bending curvatures (0, 20, and 10 mm), as it retains ∼80% of its photoresponsivity up to 500 bending cycles. Thus, our study provides a simple route to realize broadband and stable photoactivity in flexible 2D material-based devices.

Optically Reconfigurable Complementary Logic Gates Enabled by Bipolar Photoresponse in Gallium Selenide Memtransistor.

To avoid the complexity of the circuit for in-memory computing, simultaneous execution of multiple logic gates (OR, AND, NOR, and NAND) and memory behavior are demonstrated in a single device of oxygen plasma-treated gallium selenide (GaSe) memtransistor. Resistive switching behavior with RON /ROFF ratio in the range of 104 to 106 is obtained depending on the channel length (150 to 1600 nm). Oxygen plasma treatment on GaSe film created shallow and deep-level defect states, which exhibit carriers trapping/de-trapping, that lead to negative and positive photoconductance at positive and negative gate voltages, respectively. This distinguishing feature of gate-dependent transition of negative to positive photoconductance encourages the execution of four logic gates in the single memory device, which is elusive in conventional memtransistor. Additionally, it is feasible to reversibly switch between two logic gates by just adjusting the gate voltages, e.g., NAND/NOR and AND/NAND. All logic gates presented high stability. Additionally, memtransistor array (1×8) is fabricated and programmed into binary bits representing ASCII (American Standard Code for Information Interchange) code for the uppercase letter "N". This facile device configuration can provide the functionality of both logic and memory devices for emerging neuromorphic computing.

Filamentary and Interface-Type Memristors Based on Tantalum Oxide for Energy-Efficient Neuromorphic Hardware.

To implement artificial neural networks (ANNs) based on memristor devices, it is essential to secure the linearity and symmetry in weight update characteristics of the memristor, and reliability in the cycle-to-cycle and device-to-device variations. This study experimentally demonstrated and compared the filamentary and interface-type resistive switching (RS) behaviors of tantalum oxide (Ta2O5 and TaO2)-based devices grown by atomic layer deposition (ALD) to propose a suitable RS type in terms of reliability and weight update characteristics. Although Ta2O5 is a strong candidate for memristor, the filament-type RS behavior of Ta2O5 does not fit well with ANNs demanding analog memory characteristics. Therefore, this study newly designed an interface-type TaO2 memristor and compared it to a filament type of Ta2O5 memristor to secure the weight update characteristics and reliability. The TaO2-based interface-type memristor exhibited gradual RS characteristics and area dependency in both high- and low-resistance states. In addition, compared to the filamentary memristor, the RS behaviors of the TaO2-based interface-type device exhibited higher suitability for the neuromorphic, symmetric, and linear long-term potentiation (LTP) and long-term depression (LTD). These findings suggest better types of memristors for implementing ionic memristor-based ANNs among the two types of RS mechanisms.

Bipolar Resistive Switching in Lanthanum Titanium Oxide and an Increased On/Off Ratio Using an Oxygen-Deficient ZnO Interlayer.

The present study pioneered an oxygen migration-driven metal to insulator transition Mott memory, a new type of nonvolatile memory using lanthanum titanium oxide (LTO). We first show the reset first bipolar property without an initial electroforming process in LTO. We used oxygen-deficient ZnO as an interlayer between LTO and a W electrode to clarify whether oxygen migration activates LTO as the Mott transition. ZnO oxygen deficiency provides oxygen ion migration paths as well as a reservoir, facilitating oxygen migration from LTO to the W electrode. Thus, including the ZnO interlayer improved oxygen migration between LTO and the W electrode, achieving a 10-fold increased on/off current ratio. The current research contributes to a better understanding of valence change Mott memory by exploring the LTO resistive switching mechanism and ZnO interlayer influences on the oxygen migration process.

Supercapacitors based on Ti3C2Tx MXene extracted from supernatant and current collectors passivated by CVD-graphene.

An ultrahigh capacity supercapacitor is fabricated using a nano-layered MXene as an active electrode material, and Ni-foil is used as a current collector. The high-quality Ti3C2Tx obtained from supernatant during etching and washing processes improves the specific capacitance significantly. As another strategy, the surface of Ni-foil is engineered by coating chemical vapor deposition-grown graphene. The graphene grown directly on the Ni-foil is used as a current collector, forming the electrode structure of Ti3C2Tx/graphene/Ni. The surface passivation of the current collectors has a high impact on charge-transfer, which in turn increases the capacitance of the supercapacitors. It is found that the capacitance of the graphene-based supercapacitors is more than 1.5 times of the capacitance without graphene. A high specific capacitance, ~ 542 F/g, is achieved at 5 mV/s scan rate based on cyclic voltammetry analysis. Also, the graphene-based supercapacitor exhibits a quasi-rectangular form in cyclic voltammetry curves and a symmetric behavior in charge/discharge curves. Furthermore, cyclic stability up to 5000 cycles is confirmed with high capacitance retention at high scan rate 1000 mV/s. A reduced series resistance with a high limit capacitance is revealed by equivalent circuit analysis with the Nyquist plot.

High performance complementary WS2 devices with hybrid Gr/Ni contacts.

Two-dimensional (2D) transition metal dichalcogenides have attracted vibrant interest for future solid-state device applications due to their unique properties. However, it is challenging to realize 2D material based high performance complementary devices due to the stubborn Fermi level pinning effect and the lack of facile doping techniques. In this paper, we reported a hybrid Gr/Ni contact to WS2, which can switch carrier types from n-type to p-type in WS2. The unorthodox polarity transition is attributed to the natural p-doping of graphene with Ni adsorption and the alleviation of Fermi level pinning in WS2. Furthermore, we realized asymmetric Ni and Gr/Ni hybrid contacts to a multilayer WS2 device, and we observed synergistic p-n diode characteristics with excellent current rectification exceeding 104, and a near unity ideality factor of 1.1 (1.6) at a temperature of 4.5 K (300 K). Lastly, our WS2 p-n device exhibits high performance photovoltaic ability with a maximum photoresponsivity of 4 × 104 A W-1 at 532 nm wavelength, that is 108 times higher than that of graphene and 50 times better than that of the monolayer MoS2 photodetector. This doping-free carrier type modulation technique will pave the way to realize high performance complementary electronics and optoelectronic devices based on 2D materials.

Enhanced electrical and broad spectral (UV-Vis-NIR) photodetection in a Gr/ReSe2/Gr heterojunction.

Vertical integration of two dimensional (2D) layered materials is indispensable in making van der Waals (vdWs) heterostructures for promising electronic and optoelectronic devices. Herein, we report excellent electrical and photoelectrical measurements where the current ON & OFF ratio of FET is increased by decreasing the temperature in the graphene/ReSe2/graphene heterojunction. We investigated the photoresponsivity in broad spectral range (UV-Vis-NIR) and achieved high photoresponsivity of 1.5 × 107 A W-1 and external quantum efficiency of ∼64% at λ = 220 nm. Further, the photovoltaic effect was examined, which significantly modulated the short circuit current (Isc) from 4.2 × 10-8 A to 2.6 × 10-7 A and open-circuit voltage (Voc) from 0.21 V to 0.44 V at different wavelengths (1064, 840, 514 and 220 nm), attributed to the photo-generation and recombination rate of the carriers. Moreover, photoresponsivity was observed near 1.2 × 106, 8.6 × 106 and 1.5 × 107 A W-1 by applying different gate biases (0, 20 and 40 V), respectively. Further, we have explored the photocurrent and photoresponsivity at different intensities of incident light (200, 260, 400, 620 and 850 µW cm-2). In addition, we calculated the rise and decay response times of photodetectors at different wavelengths and power densities, which depend upon the trap sites in the energy band of ReSe2. These devices opened up new ways to improve the performance of photodetectors from the UV to the NIR region.

Modulation of Magnetoresistance Polarity in BLG/SL-MoSe2 Heterostacks.

Two-dimensional (2D) layered materials have an atomically thin and flat nature which makes it an ultimate candidate for spintronic devices. The spin-valve junctions (SVJs), composed of 2D materials, have been recognized as unique features of spin transport polarization. However, the magnetotransport properties of SVJs are highly influenced by the type of intervening layer (spacer) inserted between the ferromagnetic materials (FMs). In this situation, the spin filtering effect at the interfaces plays a critical role in the observation of the magnetoresistance (MR) of such magnetic structures, which can be improved by using promising hybrid structure. Here, we report MR of bilayer graphene (BLG), single-layer MoSe2 (SL-MoSe2), and BLG/SL-MoSe2 heterostack SVJs. However, before annealing, BLG and SL-MoSe2 SVJs demonstrate positive MR, but after annealing, BLG reverses its polarity while the SL-MoSe2 maintains its polarity and demonstrated stable positive spin polarizations at both interfaces due to meager doping effect of ferromagnetic (FM) contacts. Further, Co/BLG/SL-MoSe2/NiFe determines positive MR, i.e., ~ 1.71% and ~ 1.86% at T = 4 K before and after annealing, respectively. On the contrary, NiFe/BLG/SL-MoSe2/Co SVJs showed positive MR before annealing and subsequently reversed its MR sign after annealing due to the proximity-induced effect of metals doping with graphene. The obtained results can be useful to comprehend the origin of polarity and the selection of non-magnetic material (spacer) for magnetotransport properties. Thus, this study established a new paragon for novel spintronic applications.

Polymer-dispersed liquid-crystal-based switchable glazing fabricated via vacuum glass coupling.

Polymer-dispersed liquid crystals (PDLCs) exhibiting transmittance switching are utilized for preserving energy and protecting privacy. Here we prepared a typical PDLC mixture from a commercially available polymer and liquid crystal with nano-beads. A wire-bar coater was used to coat the PDLC mixture on indium-tin-oxide-coated glass, and a PDLC cell was assembled by coupling another glass in a vacuum, instead of a polymer film. Uniform glass-based PDLCs were fabricated successfully with an area of 15 × 15 cm2, while an injection process with capillary action was not available for this large-scale device fabrication. The switching behavior of the cells was characterized by ramping the AC voltage, and a transmittance change of ∼70% was measured. In a typical roll-to-roll process, only flexible polymer films have been used in lamination, in which deterioration in transparency occurs over the course of time, reducing the efficiency. In this study, to improve the optical properties, PDLC switchable glazing is fabricated directly onto glass substrates instead of onto plastic polymers. This PDLC switchable glazing, exhibiting low haziness and wide-angle vision, can be fabricated at a large scale by a vacuum-coupling process, with potential use as glass windows for energy-efficient buildings.

Effect of Ti3C2T x MXenes etched at elevated temperatures using concentrated acid on binder-free supercapacitors.

The effect of Ti3C2T x MXene etched at different temperatures (25 °C, 50 °C, and 80 °C) on the capacitance of supercapacitors without the use of conducting carbon-black or a binder was studied. The MXene etched using concentrated HCl acid (12 M)/LiF was used as an active electrode and Ni-foil as a current collector. It was observed that the elevated etching temperature facilitates the etching of the MAX phase and the exfoliation of MXene layers. However, this led to the formation of additional functional groups at the MXene surface as the temperature was increased to 80 °C. The specific capacitance of Ti3C2T x -based supercapacitors increased from 581 F g-1 for MXene etched at 25 °C to 657 F g-1 for those etched at 50 °C at the scan rate of 2 mV s-1. However, the specific capacitance reduced to 421 F g-1 as the etching temperature was increased to 80 °C at the same scan rate. The supercapacitors based on MXenes etched at the intermediate temperature (50 °C) exhibited higher specific capacitance in a wide range of scan rate, symmetry in charge/discharge curves, high cyclic stability at a scan rate of 1000 mV s-1 for up to 3000 cycles. The electrochemical impedance spectroscopy studies indicated low series resistance, reduced charge-transfer resistance, and decreased Warburg impedance for the supercapacitor based on the MXene etched at the intermediate temperature.

Quartz tuning fork based three-dimensional topography imaging for sidewall with blind features.

Atomic force microscopy has a tremendous number of applications in a wide variety of fields, particularly in the semiconductor area for the 3D-stacked device. Imaging three-dimensional (3D) structures with blind features has progressively become a critical technique. Recently, a 3D-atomic force microscopy (AFM) technique has been proposed to image 3D features, especially those having sharp apices, like silicon pillars. However, the scanning strategy has drawbacks, such as long scanning time, and unstable operation, based on the premature algorithm. Herein, an improved 3D-AFM algorithm is reported that overcomes the aforementioned problems by an intelligent 3D scanning algorithm that incorporates sidewall history tracking, troubleshooting for sharp sidewall and sticking, and reactive direction adjustment. The proposed algorithm enables the 3D imagery of ZnO nano-rods and silicon nano-pillars to be achieved by using a high aspect-ratio multiwall carbon nanotube-based AFM probe, without time-consuming disorientation. This study establishes a method to construct a 3D image of arbitrary shape in reduced scanning time.

Twist-Angle-Dependent Optoelectronics in a Few-Layer Transition-Metal Dichalcogenide Heterostructure.

Lattice matching has been supposed to play an important role in the coupling between two materials in a vertical heterostructure (HS). To investigate this role, we fabricated a heterojunction device with a few layers of p-type WSe2 and n-type MoSe2 with different crystal orientation angles. The crystal orientations of WSe2 and MoSe2 were estimated using high-resolution X-ray diffraction. Heterojunction devices were fabricated with twist angles of 0, 15, and 30°. The I- V curve of the sample with the twist angle of 0° under the dark condition showed a diodelike behavior. The strong coupling due to lattice matching caused a well-established p-n junction. In cases of 15 and 30° samples, the van der Waals gap was built because of lattice mismatching, which resulted in the formation of a potential barrier. However, when the light-emitting diode light of 365 nm (3.4 eV) was illuminated, it was possible for excited electrons and holes to jump beyond the potential barrier and the current flowed well in both forward and reverse directions. The effects of the twist angle were analyzed by spectral responsivity and external quantum efficiency, where it was found that the untwisted HS exhibited higher sensitivity under IR illumination, whereas the twisting effect was not noticeable under UV illumination. From photoluminescence and Raman spectroscopy studies, it was confirmed that the twisted HS showed a weak coupling because of the lattice mismatch.

Acrylate-assisted fractal nanostructured polymer dispersed liquid crystal droplet based vibrant colored smart-windows.

We have studied liquid crystals (LCs) and acrylate-assisted thiol-ene compositions to synthesize dye based colorful polymer dispersed liquid crystals (PDLCs) without using a photo-initiator for smart-windows applications. A typical PDLC mixture was prepared by mixing LCs with UV-curable monomers, which included triethylene glycol diacrylate (TEGDA), trimethylolpropane diallyl ether (TMPDE, di-functional ene monomer), trimethylolpropane tris(3-mercaptopropionate) (TMPTMP, a thiol as a cross-linker), and a dichroic dye. The ratios of the TMPDE/TMPTMP and the LCs/TEGDA showed significant effects in altering the properties of the UV-cured PDLCs. During the curing process, the monomers polymerize and led to the encapsulation of the LCs in the form of interesting fractal nanostructures by a polymerization induced phase separation process. The switching time, electro-optical properties, power consumption, and ageing of the fabricated PDLCs were investigated. It was possible to achieve a 70-80% contrast (ΔT) at a voltage difference of ∼70 V with a fast switching time (τ) as low as < 20 milliseconds (ms) and low power consumption. These PDLCs had a low threshold voltage that ranged between 10 and 20 V. The sustainability of the fabricated UV-cured PDLCs was analyzed for up to 90 days, and the PDLCs were observed to be stable.

Comparison of Electrical and Photoelectrical Properties of ReS2 Field-Effect Transistors on Different Dielectric Substrates.

As one of the newly discovered transition-metal dichalcogenides (TMDs), rhenium disulfide (ReS2) has been investigated mostly because of its unique characteristics such as the direct band gap nature even in bulk form, which is not prominent in other TMDs (e.g., MoS2, WSe2, etc.). However, this material possesses a low mobility and an on/off ratio, which restrict its usage in high-speed and fast switching applications. Low mobilities or on/off ratios can also be caused by substrate scattering as well as environmental effects. In this study, we used few-layer ReS2 (FL-ReS2) as a channel material to investigate the substrate-dependent mobility, current on/off ratio, Schottky barrier height (SBH), and trap density of states of different dielectric substrates. The hexagonal boron nitride (h-BN)/FL-ReS2/h-BN structure was observed to exhibit a high mobility of 45 cm2 V-1 s-1, current on/off ratio of about 107, the lowest SBH of about 12 mV at a zero back-gate voltage ( Vbg), and a low trap density of states of about 5 × 1013 cm-3. These quantities are reasonably superior compared to the FL-ReS2 devices on SiO2 substrates. We also observed a nearly 5-fold improvement in the photoresponsivity and external quantum efficiency values for the FL-ReS2 devices on h-BN substrates. We believe that the photonic characteristics of TMDs can be improved by using h-BN as the substrate and capping layer.

Gate Tunable Transport in Graphene/MoS2/(Cr/Au) Vertical Field-Effect Transistors.

Two-dimensional materials based vertical field-effect transistors have been widely studied due to their useful applications in industry. In the present study, we fabricate graphene/MoS2/(Cr/Au) vertical transistor based on the mechanical exfoliation and dry transfer method. Since the bottom electrode was made of monolayer graphene (Gr), the electrical transport in our Gr/MoS2/(Cr/Au) vertical transistors can be significantly modified by using back-gate voltage. Schottky barrier height at the interface between Gr and MoS2 can be modified by back-gate voltage and the current bias. Vertical resistance (Rvert) of a Gr/MoS2/(Cr/Au) transistor is compared with planar resistance (Rplanar) of a conventional lateral MoS2 field-effect transistor. We have also studied electrical properties for various thicknesses of MoS2 channels in both vertical and lateral transistors. As the thickness of MoS2 increases, Rvert increases, but Rplanar decreases. The increase of Rvert in the thicker MoS2 film is attributed to the interlayer resistance in the vertical direction. However, Rplanar shows a lower value for a thicker MoS2 film because of an excess of charge carriers available in upper layers connected directly to source/drain contacts that limits the conduction through layers closed to source/drain electrodes. Hence, interlayer resistance associated with these layers contributes to planer resistance in contrast to vertical devices in which all layers contribute interlayer resistance.