Two-dimensional Devices Research Articles

H-BN-assisted-transferred metal contacts to InSe for twodimensional multifunctional electronic devices

Abstract Metal contacts to two-dimensional semiconductors play a crucial role in determining the electrical performance of the electronic devices. However, traditional three-dimensional metal deposition processes will bring damage to two-dimensional semiconductors and cause significant Fermi-level-pinning effects. In this work, we report a hexagonal boron nitride (h-BN)-assisted-transferred method for metal contacts to few-layered InSe for construction of two-dimensional functional electronic devices. Using transferred Pt electrodes as the contact, p-type dominated ambipolar conduction behavior with the hole Schottky barrier height (SBH) approaching 0 meV was observed in field-effect transistors (FETs) based on multilayered InSe. Based on this, using a dual-gate modulating method, multiple types of InSe homojunctions, including p-p, n-n, p-n and n-p junctions, could be constructed. For InSe p-n homojunctions, a current rectification ratio of over 104 and optoelectronic detection capabilities were achieved. Furthermore, a complementary metal-oxide-semiconductor (CMOS) inverter with an ultra-high voltage gain exceeding 60 at VDD = -1 V was constructed. Our h-BN-assistedtransferred metal contact method can be easily extended to other two-dimensional semiconductors for the construction of complementary electronic and optoelectronic devices.

Improved Thermal Dissipation in a MoS2 Field-Effect Transistor by Hybrid High-k Dielectric Layers.

Transition metal dichalcogenides like MoS2 have been considered as crucial channel materials beyond silicon to continuously advance transistor scaling down owing to their two-dimensional structure and exceptional electrical properties. However, the undesirable interface morphology and vibrational phonon frequency mismatch between MoS2 and the dielectric layer induce low thermal boundary conductance, resulting in overheating issues and impeding electrical performance improvement in the MoS2 field-effect transistors. Here, we employed hybrid high-k dielectric layers of Al2O3/HfO2 to simultaneously reduce the interfacial thermal resistance and improve device electrical performance. The enhanced contact, greater vibrational phonon overlapping region, and stronger interfacial bonding force between the top Al2O3 layer and MoS2 promote the heat removal efficiency across the interface to the substrate. Under the same input power density, the temperature profile of the MoS2 transistor on the Al2O3/HfO2 has been largely reduced compared to that of the device on HfO2, with a maximum reduction of 49.5 °C. In addition, the field-effect mobility and current of MoS2 devices on the Al2O3/HfO2 high-k dielectric layers have been significantly improved, attributed to the depressed electron scattering and trap states at the interface. The design of the hybrid high-k dielectric layers provides an efficient solution to simultaneously improve the thermal and electrical performance of the two-dimensional devices.

Ferroelectric Polarization Enhanced Optoelectronic Synaptic Response of a CuInP2S6 Transistor Structure.

Neuromorphic computing can simulate brain function and is a pivotal element in next-generation computing, providing a potential solution to the limitations brought by the von Neumann bottleneck. Optoelectronic synaptic devices are highly promising tools for simulating biomimetic nervous systems. In this study, we developed an optoelectronic neuromorphic device with a transistor structure constructed using ferroelectric CuInP2S6. Essential synaptic behaviors in this device are observed in response to light and electrical stimuli. The optoferroelectric coupling is revealed, and the highly tunable gate modulation of the charge carrier is realized in a single device. On this basis, the light adaptation of the biological eyes and smarter Pavlovian dogs was implemented successfully and enhanced by ferroelectric polarization. The gate voltage application promotes the migration of additional Cu+ ions in the in-plane direction, thus enhancing the synaptic performance of electrical stimulation. Meanwhile, the processing ability of convolutional kernel noise images in ferroelectric devices has been achieved. Our results offer the important observation and application of ferroelectric polarization-enhanced synaptic properties of a transistor structure and have great potential in promoting the development of two-dimensional van der Waals materials and devices.

Thermal transport of flexural phonons in a rectangular plate

The quantum thermal transport of elastic excitations through a two-dimensional elastic waveguide between two thermal reservoirs is studied. We solve the classical Kirchhoff–Love equation for rectangular plates and explore the dispersion relation for both the symmetric and antisymmetric solutions. Then, we study the phonon transport of these modes within the second quantization framework by analyzing the mean quadratic displacement, from which the energy density current, the temperature field, and conductance are determined. We identify the relevant modes contributing to thermal transport and explore the average temperature difference to reach the high-temperature limit. We expect our results to pave the way for understanding phonon-mediated thermal transport in two-dimensional mesoscopic quantum devices.

Dual-Mode Reconfigurable Split-Gate Logic Transistor through Van der Waals Integration.

As silicon-based transistors approach their physical size limitations, two-dimensional material-based reconfigurable functional electronic devices are considered the most promising novel device architectures beyond Moore strategies. While these devices have garnered significant attention, they often require complex device fabrication processes and extra electric fields. Additionally, the device performance is usually limited by the metal-semiconductor interface properties. In this Letter, we have constructed a reconfigurable logic device based on a WSe2 transistor with a nanofloating gate and split-gates through van der Waals integration. This device achieves a small Schottky barrier height due to the van der Waals contacts. By varying the split-gate biases, we can realize volatile reconfigurable homojunctions as well as AND, OR, NOR, and NAND logic operations with just a single device. Furthermore, with the charge trapping effect of nanofloating gate, we can also achieve nonvolatile reconfigurable homojunctions, as well as AND and OR logic operations. The volatile and nonvolatile logic operations are similar to the short-term plasticity and long-term plasticity, respectively, of synapses in the human brain. This work offers a potential approach for creating novel reconfigurable functional electronic devices with a simple fabrication process and low cost.

Impact of Atomic Defects on Water Contact Angle of 2D Molybdenum Disulfide Surfaces.

Interfacial dynamics within nanofluidic systems are crucial for applications like water desalination and osmotic energy harvesting. Understanding these dynamics can inform the rational optimization of two-dimensional (2D) materials and devices for such applications. This study explores the wetting behavior of realistic 2D MoS2 surfaces incorporating vacancies and atomic steps, known as atomic defects. We employ a combined density functional theory (DFT) and molecular dynamics (MD) computational approach to elucidate the influence of atomic defects on the MoS2-water interface. DFT calculations are utilized to determine the charge distribution within MoS2. Subsequently, free energy calculations are obtained through MD simulations of the MoS2-water interface. Our findings underscore the importance of incorporating atomic defects into MoS2 surfaces for accurate water contact angle (WCA) predictions in nanofluidic simulations, particularly when using Abal et al. force field parameters. However, the force field developed by Liu et al. yielded more accurate results for pristine MoS2 surfaces. While these parameters provide reliable outcomes for pristine MoS2 surfaces, their application to surfaces with defects may lead to underestimation of WCA. This highlights the critical need for realistic surface representations in nanofluidic modeling to accurately capture the complex interactions between water and MoS2 materials.

Excimer-ultraviolet-lamp-assisted selective etching of single-layer graphene and its application in edge-contact devices

Since the discovery of graphene and its remarkable properties, researchers have actively explored advanced graphene-patterning technologies. While the etching process is pivotal in shaping graphene channels, existing etching techniques have limitations such as low speed, high cost, residue contamination, and rough edges. Therefore, the development of facile and efficient etching methods is necessary. This study entailed the development of a novel technique for patterning graphene through dry etching, utilizing selective photochemical reactions precisely targeted at single-layer graphene (SLG) surfaces. This process is facilitated by an excimer ultraviolet lamp emitting light at a wavelength of 172 nm. The effectiveness of this technique in selectively removing SLG over large areas, leaving the few-layer graphene intact and clean, was confirmed by various spectroscopic analyses. Furthermore, we explored the application of this technique to device fabrication, revealing its potential to enhance the electrical properties of SLG-based devices. One-dimensional (1D) edge contacts fabricated using this method not only exhibited enhanced electrical transport characteristics compared to two-dimensional contact devices but also demonstrated enhanced efficiency in fabricating conventional 1D-contacted devices. This study addresses the demand for advanced technologies suitable for next-generation graphene devices, providing a promising and versatile graphene-patterning approach with broad applicability and high efficiency.

A Mid-Infrared Perfect Metasurface Absorber with Tri-Band Broadband Scalability.

Metasurfaces have emerged as a unique group of two-dimensional ultra-compact subwavelength devices for perfect wave absorption due to their exceptional capabilities of light modulation. Nonetheless, achieving high absorption, particularly with multi-band broadband scalability for specialized scenarios, remains a challenge. As an example, the presence of atmospheric windows, as dictated by special gas molecules in different infrared regions, highly demands such scalable modulation abilities for multi-band absorption and filtration. Herein, by leveraging the hybrid effect of Fabry-Perot resonance, magnetic dipole resonance and electric dipole resonance, we achieved multi-broadband absorptivity in three prominent infrared atmospheric windows concurrently, with an average absorptivity of 87.6% in the short-wave infrared region (1.4-1.7 μm), 92.7% in the mid-wave infrared region (3.2-5 μm) and 92.4% in the long-wave infrared region (8-13 μm), respectively. The well-confirmed absorption spectra along with its adaptation to varied incident angles and polarization angles of radiations reveal great potential for fields like infrared imaging, photodetection and communication.

Unlocking High-Performance, Ultra-Low Power van der Waals Photo-Transistors: Toward Back-End-of-Line in-Sensor Machine Vision Applications.

Recent reports on machine learning and machine vision (MV) devices have demonstrated the potential of two-dimensional (2D) materials and devices. Yet, scalable 2D devices are being challenged by contact resistance and Fermi level pinning (FLP), power consumption, and low-cost CMOS compatible lithography processes. To enable CMOS + 2D, it is essential to find a proper lithography strategy that can fulfill these requirements. Here, we explored a modified van der Waals (vdW) deposition lithography and demonstrated a relatively new class of van der Waals field effect transistors (vdW-FETs) based on 2D materials. This lithography strategy enabled us to unlock high-performance devices evident by high current on-off ratio (Ion/Ioff), high turn-on current density (Ion), and weak FLP. We utilized this approach to demonstrate a gate-tunable near-ideal diode using a MoS2/WSe2 heterojunction with an ideality factor of ∼1.65 and current rectification of 102. We finally demonstrated a highly sensitive, scalable, and ultralow power phototransistor using a MoS2/WSe2 vdW-FET for back-end-of-line integration. Our phototransistor exhibited the highest gate-tunable photoresponsivity achieved to date for white light detection with ultralow power dissipation, enabling ultrasensitive optoelectronic applications such as in-sensor MV. Our approach showed the great potential of modified vdW deposition lithography for back-end-of-line CMOS + 2D applications.

2D Reconfigurable Memory Device Enabled by Defect Engineering for Multifunctional Neuromorphic Computing.

In this era of artificial intelligence and Internet of Things, emerging new computing paradigms such as in-sensor and in-memory computing call for both structurally simple and multifunctional memory devices. Although emerging two-dimensional (2D) memory devices provide promising solutions, the most reported devices either suffer from single functionalities or structural complexity. Here, this work reports a reconfigurable memory device (RMD) based on MoS2/CuInP2S6 heterostructure, which integrates the defect engineering-enabled interlayer defects and the ferroelectric polarization in CuInP2S6, to realize a simplified structure device for all-in-one sensing, memory and computing. The plasma treatment-induced defect engineering of the CuInP2S6 nanosheet effectively increases the interlayer defect density, which significantly enhances the charge-trapping ability in synergy with ferroelectric properties. The reported device not only can serve as a non-volatile electronic memory device, but also can be reconfigured into optoelectronic memory mode or synaptic mode after controlling the ferroelectric polarization states in CuInP2S6. When operated in optoelectronic memory mode, the all-in-one RMD could diagnose ophthalmic disease by segmenting vasculature within biological retinas. On the other hand, operating as an optoelectronic synapse, this work showcases in-sensor reservoir computing for gesture recognition with high energy efficiency.

Extraordinary photoexcitation of semimetal 1T'-MoTe2 inducing ultrafast charge transfer in lateral 2D homojunction

Exploring novel and more efficient photoexcitation transition mechanisms in two-dimensional transition metal dichalcogenides (TMDCs) is crucial for the advancement of high-performance optoelectronic devices. In this study, an extraordinary photoluminescence (PL) phenomenon is discovered that originates from a vertical transition between specific bands in the X-point energy valley of K-space in multilayer Weyl semi-metal monoclinic (1T') MoTe2 without a gap structure. This effective transition is independent of the bandgap and is unaffected by the number of layers in 1T'-MoTe2, breaking the limitations of traditional TMDCs semiconductor materials and promoting the development of advanced two-dimensional (2D) semimetal-based optoelectronic devices. In a lateral multilayer 1T'-MoTe2-2H hetero-phase homojunction, a record ultrafast transfer of photogenerated charges up to 25 fs is achieved. The highly efficient interband transition, small conduction band energy level difference (less than 100 meV), and exceptionally strong e-p coupling synergistically promote the ultrafast transfer of photo-generated charges. Together with the merits of multilayer 1T'-MoTe2 such as higher carrier densities and lower resistance, these findings open the door to potentially ultra-high performance optoelectronic applications.

Research on the robust electrical contact properties and favorable transport characteristics of two-dimensional WB4/MoSi2N4 van der Waals heterostructures

Ensuring optimal interface contact performance is crucial for achieving low-resistance ohmic contact in the design of two-dimensional (2D) electronic devices. In this study, we systematically investigate the contact properties of van der Waals (vdW) heterojunctions formed by compositing the semi-metal WB4 with Dirac cones and the semiconductor MoSi2N4 through first-principles calculations. A thorough investigation has been carried out on the electronic structure and transport characteristics at the interface. Our research findings indicate that the WB4/MoSi2N4 combination demonstrates robust ohmic contact performance, maintaining ohmic or near-ohmic p-type Schottky contacts over a wide range when exposed to electric field, varying layer spacing, and biaxial strain. This unique characteristic is associated with the Fermi level pinning (FLP), where there are gap states present at the interface. Here, the FLP plays a positive role in maintaining ohmic contact. In addition, different derivatives of MoSi2N4 are combined with WB4 to create heterostructures and study the changes in contact performance. Our research shows that the robust ohmic contact of WB4/MoSi2N4 will have excellent prospects for application in future electronic devices.

Damage-free dry transfer method using stress engineering for high-performance flexible two- and three-dimensional electronics.

Advanced transfer printing technologies have enabled the fabrication of high-performance flexible and stretchable devices, revolutionizing many research fields including soft electronics, optoelectronics, bioelectronics and energy devices. Despite previous innovations, challenges remain, such as safety concerns due to toxic chemicals, the expensive equipment, film damage during the transfer process and difficulty in high-temperature processing. Thus a new transfer printing process is needed for the commercialization of high-performance soft electronic devices. Here we propose a damage-free dry transfer printing strategy based on stress control of the deposited thin films. First, stress-controlled metal bilayer films are deposited using direct current magnetron sputtering. Subsequently, mechanical bending is applied to facilitate the release of the metal bilayer by increasing the overall stress. Experimental and simulation studies elucidate the stress evolution mechanisms during the processes. By using this method, we successfully transfer metal thin films and high-temperature-treated oxide thin films onto flexible or stretchable substrates, enabling the fabrication of two-dimensional flexible electronic devices and three-dimensional multifunctional devices.

Electric-field-controlled electronic structures and quantum transport in monolayer InSe nanoribbons

Electronic structures and quantum transport properties of the monolayer InSe nanoribbons are studied by adopting the tight-binding model in combination with the lattice Green function method. Besides the normal bulk and edge electronic states, a unique electronic state dubbed as edge-surface is found in the InSe nanoribbon with zigzag edge type. In contrast to the zigzag InSe nanoribbon, a singular electronic state termed as bulk-surface is observed along with the normal bulk and edge electronic states in the armchair InSe nanoribbons. Moreover, the band gap, the transversal electron probability distributions in the two sublayers, and the electronic state of the topmost valence subband can be manipulated by adding a perpendicular electric field to the InSe nanoribbon. Further study shows that the charge conductance of the two-terminal monolayer InSe nanoribbons can be switched on or off by varying the electric field strength. In addition, the transport of the bulk electronic state is delicate to even a weak disorder strength, however, that of the edge and edge-surface electronic states shows a strong robustness against to the disorders. These findings may be helpful to understand the electronic characteristics of the InSe nanostructures and broaden their potential applications in two-dimensional nanoelectronic devices as well.

Progress on the program of Si-compatible two-dimensional semiconductor materials and devices

Progress on the program of Si-compatible two-dimensional semiconductor materials and devices

From flat to folded: An instrument-free solution for chemical and biological paper-based sensing using A-PAP pen technology

Having economical, flexible, disposable and readily manufacturable devices for everyday sensing applications is of paramount importance. We report a novel and cost-effective technique for fabricating paper-based devices using an Advanced PAP (A-PAP) pen, which is capable of withstanding typical aqueous solutions and organic solvents. The quick fabrication process does not require any sophisticated instrumentation or a heating step, making it a promising technology for resource-limited settings. Using an A-PAP pen, we have fabricated two-dimensional (2D) paper-based devices for chemical detection of heavy metal and nitrite. We have also demonstrated the versatility of fabrication technique for biological sensing using 2D lateral flow paper-based devices for the detection of dopamine. Furthermore, the technique is also validated for fabricating complex three-dimensional (3D) paper-based devices using a paper origami technique for heavy metals sensing. The ready-to-use devices can be fabricated in seconds, making them convenient for on-the-spot testing. Overall, this technique provides a valuable tool for creating affordable, efficient, and accessible chemical and biological testing solutions.

Hole-Doped Nonvolatile and Electrically Controllable Magnetism in van der Waals Ferroelectric Heterostructures

Electrical control of magnetism in van der Waals semiconductors is a promising step towards development of two-dimensional spintronic devices with ultralow power consumption for processing and storing information. Here, we propose a design for two-dimensional van der Waals heterostructures (vdWHs) that can host ferroelectricity and ferromagnetism simultaneously under hole doping. By contacting an InSe monolayer and forming an InSe/In2Se3 vdWH, the switchable built-in electric field from the reversible out-of-plane polarization enables robust control of the band alignment. Furthermore, switching between the two ferroelectric states (P ↑ and P ↓) of hole-doped In2Se3 with an external electric field can interchange the ON and OFF states of the nonvolatile magnetism. More interestingly, doping concentration and strain can effectively tune the magnetic moment and polarization energy. Therefore, this provides a platform for realizing multiferroics in ferroelectric heterostructures, showing great potential for use in nonvolatile memories and ferroelectric field-effect transistors.

High Spatial Resolution 2D Imaging of Current Density and Pressure for Graphene Devices under High Pressure Using Nitrogen-Vacancy Centers in Diamond.

Current density imaging is helpful for discovering interesting electronic phenomena and understanding carrier dynamics, and by combining pressure distributions, several pressure-induced novel physics may be comprehended. In this work, noninvasive, high-resolution two-dimensional images of the current density and pressure gradient for graphene ribbon and hBN-graphene-hBN devices are explored using nitrogen-vacancy (NV) centers in diamond under high pressure. The two-dimensional vector current density is reconstructed by the vector magnetic field mapped by the near-surface NV center layer in the diamond. The current density images accurately and clearly reproduce the complicated structure and current flow of graphene under high pressure. Additionally, the spatial distribution of the pressure is simultaneously mapped, rationalizing the nonuniformity of the current density under high pressure. The current method opens a significant new avenue to investigate electronic transport and conductance variations in two-dimensional materials and electrical devices under high pressure as well as for nondestructive evaluation of semiconductor circuits.

Biaxila strain modulated high anisotropic gas-sensing performance of C5N-based two-dimensional devices: A first-principles study

Two-dimensional carbon nitride materials have been widely used in many applications such as device fabrication, gas adsorption and separation due to their abundant element resources, high physicochemical stability and excellent electronic properties. In this paper, density functional theory and non-equilibrium Green's function method are used to study the electronic structure, transport characteristics and gas sensitivity of C5N-based structures. The results show that the electron transport exhibits obvious anisotropy, in which the electron transport in the armchair direction is more conductive than that in the zigzag direction. It is worth noting that the negative differential resistance effect exists in both directions. Furthermore, the transport and sensing characteristics of inorganic molecules (NO, CO, NO2, SO2, and NH3) adsorbed on the C5N monolayer are studied. The results show that CO, SO2 and NH3 exist on the surface of C5N in the form of physical adsorption, while NO and NO2 adhere to the surface of C5N in the form of chemical adsorption. The designed C5N gas sensor exhibits high sensitivity to NO and NO2 molecules, reaching 81 % sensitivity to NO2 at a 0.1 V bias voltage. Finally, the effect of strain on the adsorption properties of gas sensing devices is studied. Studies have shown that the application of -4 % strain in the armchair direction significantly increases the current of NO and NO2, significantly improving the performance of the gas sensor. Whether strain is applied to the device or gas adsorption, C5N materials always maintain significant anisotropy. This study shows that C5N is a highly anisotropic and sensitive two-dimensional material, which has broad application potential in the field of electronic properties and gas sensing.

Thermal bridging effect enhancing heat transport across graphene interfaces with pinhole defects

Interfacial thermal conductance (G) is of critical significance to the efficient thermal management of two-dimensional (2D) material devices. Despite the importance of defects engineering in tuning G, the mechanisms of heat transport across defective graphene interfaces remain unclear. In this study, we have identified and demonstrated the origins of the enhanced heat transport across pinhole defective graphene through our ultrafast pump-probe measurements and molecular dynamics (MD) simulations. In prior work, the enhanced G across defective graphene interfaces was commonly attributed to the improved overlap of phonon density of states (DOS) or interfacial coupling strength. We, however, observe a remarkable 2.5-fold increase in heat conduction and a distinctly different temperature dependence of G for defective graphene with the same superstrate and substrate material, compared to pristine graphene. In contrast, interfaces with different superstrate and substrate materials show only minor changes (<15%) in thermal conductance after introducing defects in the graphene layer. Through careful analysis of our MD simulations for various defective graphene interfaces, we conclude that, contradictory to common beliefs, it is the formation of direct contact thermal bridge, instead of the improvement in the phonon DOS overlap or interfacial coupling strength, that has a decisive effect and promotes heat transport across defective graphene interfaces. The differing impacts of the thermal bridge on G of defective graphene sandwiched by layers of the same and different materials are primarily attributed to the varying coupling strength between the substrate and superstrate. Our work provides important insights and physical understandings of the mechanisms of heat conduction across defective graphene interfaces.