Search

Abstract C–H bond activation enables the facile synthesis of new chemicals. While C–H activation in short-chain alkanes has been widely investigated, it remains largely unexplored for long-chain organic molecules. Here, we report light-driven C–H activation in complex organic materials mediated by 2D transition metal dichalcogenides (TMDCs) and the resultant solid-state synthesis of luminescent carbon dots in a spatially-resolved fashion. We unravel the efficient H adsorption and a lowered energy barrier of C–C coupling mediated by 2D TMDCs to promote C–H activation and carbon dots synthesis. Our results shed light on 2D materials for C–H activation in organic compounds for applications in organic chemistry, environmental remediation, and photonic materials.

Abstract 3D neuromorphic hardware system is first demonstrated in neuromorphic application as on‐chip level by integrating array devices with CMOS circuits after wafer bonding (WB) and interconnection process. The memory window of synaptic device is degraded after WB and 3 Dimesional (3D) integration due to process defects and thermal stress. To address this degradation, Ag diffusion in materials of Ta2O5 and HfO2 is studied in a volatile memristor, furthermore, the interconnection and gate metal Ru are investigated to reduce defective traps of gate interface in non‐volatile memory devices. As a result, a memory window is improved over 106 in both types of devices. Improved and 3D integrated 12 × 14 array devices are identified in the synaptic characteristics according to the change of the synaptic weight from the interconnected Test Element Group (TEG) of the Complementary Metal Oxide Semiconductor (CMOS) circuits. The trained array devices present recognizable image of letters, achieving an accuracy rate of 92% when utilizing a convolutional neural network, comparing the normalized accuracy of 93% achieved by an ideal synapse device. This study proposes to modulate the memory windows up to 106 in an integrated hardware‐based neural system, considering the possibility of device degradation in both volatile and non‐volatile memory devices demonstrated by the hardware neural system.

A fully depleted silicon‐on‐insulator (FDSOI) metal‐oxide‐semiconductor field‐effect transistors (MOSFETs) device is investigated as for an electronic synapse emulating the synaptic functions of the human brain with stable characteristics. Gate‐last processed FDSOI MOSFET with a high‐k/metal gate stack features a memory window of 103. Synaptic conductance is stably regulated by utilizing the FDSOI MOSFET, which offers the advantage of mitigating leakage current when compared to bulk Si MOSFET. Short‐ and long‐term plasticity are investigated by applying engineered pulse, verifying the long‐term synaptic properties of pattern recognition processes. With controllable synaptic conductance, the trade‐off between conductance change and linearity regarding the recognition rate is evaluated, attaining a recognition rate of 0.83. To verify the pre‐ and post‐synaptic weights within a real hardware‐based neuromorphic system, 5 × 6 FDSOI field‐effect transistor (FET) synapse array is interconnected to 10 × 10 leaky integrate‐and‐fire (LIF) neuron array. The synaptic plasticity of FDSOI MOSFET in post‐neurons following neuron firing in the neuron device is successfully demonstrated. These results indicate that FDSOI MOSFET devices could be applicable as synapse devices due to controllability and capability to realize signal transmissions and self‐learning processes simultaneously and used to mimic a synapse neuron network system by configuring a hardware system interconnected with the LIF neuron.

Abstract The layered semiconductor In2Se3 has a low temperature crystalline–crystalline (α → β) phase transformation with distinct electrical properties that make it a promising candidate for phase change memory. Here, using scanning tunneling microscopy, correlative in situ micro‐Raman, and electrical measurements, it is shown that the β phase can persist in bulk crystals at room temperature in non‐oxidative environments. Of particular note, the stability of β phase crystals in ambient conditions under encapsulation of graphene and similar passivation layers, is reported for the first time. The strategy of encapsulation to ensure the persistence of β phase overlaps with efforts to passivate switching materials. It is further demonstrated that degradation from the elevated temperatures required for the phase change is slowed through examination of Raman signatures. These results demonstrate an alternative method of phase manipulation with a new stabilization of β‐In2Se3 in ambient conditions potentially extendable to other polymorphic materials, and the importance of passivation in In2Se3 memory devices.

Abstract Multiferroic materials, showing simultaneous ferroelectric and ferromagnetic orders, are considered to be promising candidates for future data storage technology however, the multiferroic phenomenon in two-dimensional (2D) materials is rarely observed. We report a simple approach to observe frequency-dependent ferroelectricity and multiferroicity in 2D Ti3C2T x MXene film at room-temperature. To study the frequency and poling effect on ferroelectricity, we performed electric polarization vs. electric field (P-E) measurement at different frequencies, measured under zero and non-zero static magnetic fields. The results not only indicate a clear frequency dependence of electric domains owing to varying time relaxation during reversal dynamic but also showed magnetic field control of electric polarization thus, confirmed the presence of strong magneto-electric (ME) coupling at room-temperature. The existence of ME coupling was attributed to the coupling between disordered electric dipoles with local spin moments as well reduced dielectric loss after heat-treatment. Moreover, the ferroelectric Ti3C2T x MXene film was employed as an active layer within the resistive data storage device that showed a stable switching behavior along with improved on/off ratio in comparison to non-ferroelectric Ti3C2T x active layer. The unique multiferroic behavior along with ferroelectric-tuned data storage devices reported here, will help understand the intrinsic nature of 2D materials and will advance the 2D ferroelectric data storage industry.

Designing biocompatible and flexible electronic devices for neuromrophic applications remains a challenge. Here, Kireev et al. propose graphene-based artificial synaptic transistors with low-energy switching, long-term potentiation, and metaplasticity for future bio-interfaced neural networks.

Abstract Graphene electronic tattoos (GETs) have recently emerged as unique tools for personalized healthcare. The monolayer GETs have been used to monitor human electrophysiological signals, including brain, heart, and muscle activities, skin temperature, and hydration level. However, a few drawbacks of the earlier GETs hindered their perception by clinical and biomedical experts: they were not permeable to sweat, and the tattoo performance varied greatly. In this work, we introduce GETs 2.0: the skin wearable tattoo sensors with superior electrical properties, permeability to sweat, and robustness. We report on the categorical analysis of the graphene tattoos of different layer constitutions. When stacking the graphene monolayers within a single tattoo, we see a drastic enhancement in their electronic properties. The older monolayer GETs were susceptive to minor growth- or transfer-related discrepancies, resulting in highly scattered electrical properties. In this work, the GETs 2.0 with the addition of graphene nanoscrolls (GNS) or multilayer (2 L and 3 L) graphene structures exhibit 3.5-fold decreased sheet resistance, 2.5-fold lower skin impedance, and 5-fold reduced standard deviations of these values. In addition, we introduced holes into the tattoo, enabling healthy sweat evaporation without a substantial decrease in electrical properties. Furthermore, we show that microholes allow for advanced biplanar contact with graphene tattoos. Finally, we show that multilayer GETs 2.0 can be used as efficient skin-wearable electronic heaters, exhibiting heating efficiency of ~6 mW/°C.

Abstract Monolayer molybdenum disulfide has been previously discovered to exhibit non-volatile resistive switching behavior in a vertical metal-insulator-metal structure, featuring ultra-thin sub-nanometer active layer thickness. However, the reliability of these nascent 2D-based memory devices was not previously investigated for practical applications. Here, we employ an electron irradiation treatment on monolayer MoS2 film to modify the defect properties. Raman, photoluminescence, and X-ray photoelectron spectroscopy measurements have been performed to confirm the increasing amount of sulfur vacancies introduced by the e-beam irradiation process. The statistical electrical studies reveal the reliability can be improved by up to 1.5× for yield and 11× for average DC cycling endurance in the devices with a moderate radiation dose compared to unirradiated devices. Based on our previously proposed virtual conductive-point model with the metal ion substitution into sulfur vacancy, Monte Carlo simulations have been performed to illustrate the irradiation effect on device reliability, elucidating a clustering failure mechanism. This work provides an approach by electron irradiation to enhance the reliability of 2D memory devices and inspires further research in defect engineering to precisely control the switching properties for a wide range of applications from memory computing to radio-frequency switches.

Graphene and related two-dimensional (2D) materials have remained an active field of research in science and engineering for over fifteen years. Here, the authors investigate why the transition from laboratories to fabrication plants appears to lag behind expectations, and summarize the main challenges and opportunities that have thus far prevented the commercialisation of these materials.

Abstract Emerging Xenes, mostly group IVA and VA elemental two‐dimensional (2D) materials, have small and tunable band gaps between graphene and transition metal dichalcogenides, giving versatile electrical properties. While their microelectronic or optoelectronic properties are being extensively explored, there remains a lack of study on Xenes' uniquely advantageous thermoelectric performance. This review highlights state‐of‐the‐art experimental and theoretical progress in the thermoelectric effect and devices of IVA and VA Xenes. Vertically displaced, a.k.a. “buckled” or “puckered,” atomic arrays result in exotic and tunable electrical or thermal transport behaviors. Different from chemical doping strategies usually employed in bulk thermoelectric materials, 2D Xenes can be tuned by physical means, such as atomic layer control and quantum confinement effects. A precise and compatible platform for 2D thermoelectric effect and devices study is available via the engagement between micro/nanofabrication of 2D Xene transistors and thermal property measurement techniques. This review also reveals potential thermoelectric applications of Xenes and their compounds (Bi2Te3, Bi2Se3, etc.), such as accurate stretchable temperature sensors, fast terahertz photodetectors, and so on.

The lack of scalable, high-quality insulators is a major problem hindering the progress on electronic devices built from 2D materials. Here, the authors review the current state-of-the-art and the future prospects of suitable insulators for 2D technologies.

Electrostatic gating of 2D transistors with ionic liquids presents intrinsic limitations. Here, the authors demonstrate n-type MoS2 and p-type WSe2 transistors on a lithium-ion solid electrolyte substrate, displaying sub-threshold values approaching the ideal limit of 60 mV/dec and complementary amplifier gain of 34 with 1 V supply.

Resistive random-access memory (RRAM) devices have drawn increasing interest for the simplicity of its structure, low power consumption and applicability to neuromorphic computing. By combining analog computing and data storage at the device level, neuromorphic computing system has the potential to meet the demand of computing power in applications such as artificial intelligence (AI), machine learning (ML) and Internet of Things (IoT). Monolayer rhenium diselenide (ReSe2), as a two-dimensional (2D) material, has been reported to exhibit non-volatile resistive switching (NVRS) behavior in RRAM devices with sub-nanometer active layer thickness. In this paper, we demonstrate stable multiple-step RESET in ReSe2 RRAM devices by applying different levels of DC electrical bias. Pulse measurement has been conducted to study the neuromorphic characteristics. Under different height of stimuli, the ReSe2 RRAM devices have been found to switch to different resistance states, which shows the potentiation of synaptic applications. Long-term potentiation (LTP) and depression (LTD) have been demonstrated with the gradual resistance switching behaviors observed in long-term plasticity programming. A Verilog-A model is proposed based on the multiple-step resistive switching behavior. By implementing the LTP/LTD parameters, an artificial neural network (ANN) is constructed for the demonstration of handwriting classification using Modified National Institute of Standards and Technology (MNIST) dataset.

Abstract A pressing challenge in engineering devices with topological insulators (TIs) is that electron transport is dominated by the bulk conductance, and so dissipationless surface states account for only a small fraction of the conductance. Enhancing the surface-to-volume ratio is a common method to enhance the relative contribution of such states. In thin films with reduced thickness, the confinement results in symmetry-breaking and is critical for the experimental observation of topologically protected surface states. We employ micro-Raman and tip-enhanced Raman spectroscopy to examine three different mechanisms of symmetry breaking in Bi2Te3 TI thin films: surface plasmon generation, charge transfer, and application of a periodic strain potential. These mechanisms are facilitated by semiconducting and insulating substrates that modify the electronic and mechanical conditions at the sample surface and alter the long-range interactions between Bi2Te3 and the substrate. We confirm the symmetry breaking in Bi2Te3 via the emergence of the Raman-forbidden $${{\boldsymbol{A}}}_{{\bf{1}}{\boldsymbol{u}}}^{{\bf{2}}}$$ A1u2 mode. Our results suggest that topological surface states can exist at the Bi2Te3/substrate interface, which is in a good agreement with previous theoretical results predicting the tunability of the vertical location of helical surface states in TI/substrate heterostructures.

Wafer-scale synthesis of p-type TMD films is critical for its commercialization in next-generation electro/optoelectronics. In this work, wafer-scale intrinsic n-type WS2 films and in situ Nb-doped p-type WS2 films were synthesized through atomic layer deposition (ALD) on 8-inch α-Al2O3/Si wafers, 2-inch sapphire, and 1 cm2 GaN substrate pieces. The Nb doping concentration was precisely controlled by altering cycle number of Nb precursor and activated by postannealing. WS2 n-FETs and Nb-doped p-FETs with different Nb concentrations have been fabricated using CMOS-compatible processes. X-ray photoelectron spectroscopy, Raman spectroscopy, and Hall measurements confirmed the effective substitutional doping with Nb. The on/off ratio and electron mobility of WS2 n-FET are as high as 105 and 6.85 cm2 V-1 s-1, respectively. In WS2 p-FET with 15-cycle Nb doping, the on/off ratio and hole mobility are 10 and 0.016 cm2 V-1 s-1, respectively. The p-n structure based on n- and p- type WS2 films was proved with a 104 rectifying ratio. The realization of controllable in situ Nb-doped WS2 films paved a way for fabricating wafer-scale complementary WS2 FETs.

Supercapacitors (SCs) have attracted great attention as renewable energy storage devices due to their high power densities and cost effectiveness. In this work, a one-step method is reported to fabricate the laser scribed SC using laser reduced Polyimide (LRPI) electrodes as a substrate. An Iono-gel polymer electrolyte based on polyvinyl alcohol, potassium hydroxide and 1-Butyl-3-methyl imidazolium Bromide ([Bmim]Br) was utilized because of its wider voltage window, good ionic conductivity and better adhesion with electrode material. The assembled device exhibited an excellent specific capacitance of 2.19 mFcm−2 at a maximum current density of 0.263 mAcm−2. The energy density is measured to be 1.21 μWhcm−2, which is much higher than a usual capacitor. Given these electrochemical properties, a cost-effective one-step method and scalable approach provides a strategy to fabricate lightweight, stretchable and flexible supercapacitors for future microscale energy storage devices i.e., flexible displays, electrical sensors and wearable electronics.

MXenes present unique features as materials for energy storage; however, limited interlayer distance, and structural stability with ongoing cycling limit their applications. Here, we have developed a unique method involving incorporating Nb atoms into MXene (Ti3C2) to enhance its ability to achieve higher ionic storage and longer stability. Computational analysis using density functional theory was performed that explained the material structure, electronic structure, band structure, and density of states in atomistic detail. Nb-doped MXene showed a good charge storage capacity of 442.7 F/g, which makes it applicable in a supercapacitor. X-ray diffraction (XRD) indicated c-lattice parameter enhancement after Nb-doping in MXene (from 19.2A° to 23.4A°), which showed the effect of the introduction of an element with a larger ionic radius (Nb). Also, the bandgap changes from 0.9 eV for pristine MXene to 0.1 eV for Nb-doped MXene, which indicates that the latter has the signature of increased conductivity due to more metallic nature, in support of the experimental results. This work presents not only the effect of doping in MXene but also helps to explain the phenomena involved in changes in physical parameters, advancing the field of energy storage based on 2D materials.

The wide application of wireless communications in various technologies calls for the development of robust yet compact radio-frequency switches. Here, Kim et al. utilize MoS2 based non-volatile memristors to switch up to THz frequencies in sub µm2 areas, whilst the switches consume zero-static energy.

At a time when the scientific community is overrun with conferences, workshops, and congresses to discuss all facets of innovation, much can be learned from considering a meeting that has withstood the test of time: the Device Research Conference (DRC). The DRC has been the launching pad for many game-changing innovations, from early transistors to new electronic materials. While the conference has undergone transformations to adapt to changing times, it remains true to its roots in a way that has enabled 75 years' worth of successful technical gatherings. Remembering DRC's past provides inspiration for preserving and, we would argue, repeating the pattern laid by this historic meeting.

Herein, we studied the novel and emerging group of 2D materials namely MXene along with its nanocomposites. This work entails detailed experimental as well as computational study of the electrochemical behavior of vanadium carbide (V2CTx) MXene and MnO2-V2C nanocomposite with varying percentages of MnO2. A specific capacitance of 551.8 F/g was achieved for MnO2-V2C nanocomposite in 1 M KOH electrolyte solution, which is more than two times higher than the gravimetric capacitance of 196.5 F/g obtained for V2C. The cyclic stability achieved for the MnO2-V2C nanocomposite resulted in a retentivity of 96.5% until 5000 cycles. The c-lattice parameter achieved for MXene is 22.6 Å, which was 13.01 Å for MAX phase. The nanocomposite resulted in a c-lattice parameter of 27.2 Å, which showed that the spatial distance between the MXene layers was efficiently obtained. The method of wet etching was used for the preparation of pristine MXene and the liquid phase precipitation method was opted for the synthesis of the MnO2-V2C nanocomposite. Density functional theory calculation was exercised so as to complement the experimental results and to understand the microscopic details, such as structure stability and electronic structure. The current report presents a comprehensive experimental and computational study on 2D MXenes for future energy storage applications.

High-frequency electronics: embedded gates boost MoS2 radio frequency transistors 2D materials enable radio frequency transistors, yet the absence of a bandgap in graphene limits its maximum oscillation frequency. A team lead by Sanjay Kumar Banerjee at the University of Texas at Austin fabricated radio frequency field-effect transistors using monolayer MoS2 grown by chemical vapor deposition. The devices feature an embedded gate structure which ensures optimal gate control over the conducting channel and improves the channel-dielectric interface, whilst requiring a reduced number of fabrication steps. As a result, the device exhibits a maximum oscillation frequency as high as 11.4 GHz, an I ON/I OFF current ratio of 108, and a remarkable transconductance of 70 μS/μm, among the highest achieved so far for MoS2 devices fabricated by means of chemical vapor deposition. These results advance the state-of-the-art performance of atomically thin radio frequency transistors.

Mid-gap defects: Carriers in a trap The temporal dynamics of photo-generated electrons and holes in MoSe2 trapped by defects are revealed. While transitional metal dichalcogenides have significant potential for optoelectronic applications, samples tend to contain defects such as vacancies and impurities, most of which affect carrier mobility by inducing mid-gap states, i.e. within the bandgap. Now a team led by Yaguo Wang from the University of Texas elucidates the role of defects in samples grown by chemical vapor deposition. Femtosecond pump probe spectroscopy reveals that such defects are prone to capture (within few picoseconds) and then release (at slightly longer timescales of hundreds of picoseconds) electrons and holes. Such dynamics are intrinsic to samples grown with this particular method and possibly linked to the oxygen-associated impurities introduced during growth. This knowledge is relevant to engineering the properties of 2D materials for optoelectronics applications.

Abstract This paper reports a 100% inkjet printed transistor with a short channel of approximately 1 µm with an operating speed up to 18.21 GHz. Printed electronics are a burgeoning area in electronics development, but are often stymied by the large minimum feature size. To combat this, techniques were developed to allow for the printings of much shorter transistor channels. The small gap size is achieved through the use of silver inks with different chemical properties to prevent mixing. The combination of the short channel and semiconducting carbon nanotubes (CNT) allows for an exceptional experimentally measured on/off ratio of 106. This all inkjet printed transistor allows for the fabrication of devices using roll-to-roll methodologies with no additional overhead compared to current state of the art production methods.

Iron deficiency (ID) is the most prevalent and severe nutritional disorder globally and is the leading cause of iron deficiency anemia (IDA). IDA often progresses subtly symptomatic in children, whereas prolonged deficiency may permanently impair development. Early detection and frequent screening are, therefore, essential to avoid the consequences of IDA. In order to reduce the production cost and complexities involved in building advanced ID sensors, the devices were fabricated using a home-built patterning procedure that was developed and used for this work instead of lithography, which allows for fast prototyping of dimensions. In this article, we report the development of graphene-based field-effect transistors (GFETs) functionalized with anti-ferritin antibodies through a linker molecule (1-pyrenebutanoic acid, succinimidyl ester), to facilitate specific conjugation with ferritin antigen. The resulting biosensors feature an unprecedented ferritin detection limit of 10 fM, indicating a tremendous potential for non-invasive (e.g., saliva) ferritin detection.

Miniaturized helix antennas are integrated with drug reservoirs to function as RFID wireless tag sensors for real-time drug dosage monitoring. The general design procedure of this type of biomedical antenna sensors is proposed based on electromagnetic theory and finite element simulation. A cost effective fabrication process is utilized to encapsulate the antenna sensor within a biocompatible package layer using PDMS material, and at the same time form a drug storage or drug delivery unit inside the sensor. The in vitro experiment on two prototypes of antenna sensor-drug reservoir assembly have shown the ability to monitor the drug dosage by tracking antenna resonant frequency shift from 2.4-2.5-GHz ISM band with realized sensitivity of 1.27 μ l/MHz for transdermal drug delivery monitoring and 2.76- μ l/MHz sensitivity for implanted drug delivery monitoring.

We report the improvement of the electrical performance of field effect transistors (FETs) fabricated on monolayer chemical vapor deposited (CVD) MoS2, by applying an interacting fluoropolymer capping layer (Teflon-AF). The electrical characterizations of more than 60 FETs, after applying Teflon-AF cap, show significant improvement of the device properties and reduced device to device variation. The improvement includes: 50% reduction of the average gate hysteresis, 30% reduction of the subthreshold swing and about an order of magnitude increase of the current on-off ratio. These favorable changes in device performance are attributed to the reduced exposure of MoS2 channels to the adsorbates in the ambient which can be explained by the polar nature of Teflon-AF cap. A positive shift in the threshold voltage of all the measured FETs is observed, which translates to the more desirable enhancement mode transistor characteristics.