2D Material-based Devices Research Articles

Excimer formation in a 2D confined space

Combination of organic dyes with 2D materials can lead to integrations forming heterostructures with tunable properties, where organic dyes, with their distinct energy levels and high absorption, can enhance the performance of 2D material-based optoelectronic devices. This manuscript focuses on the confinement-induced changes of such structures containing 4,4’-(2,6-naphthalenediyl)dipyridine dications capable to form excimer species within the 2D interlayer space of synthetic saponite. The interlayer space provides an interesting microenvironment enabling to control optical properties of the intercalated organic molecules by either varying their amount or expanding the interlayer space via swelling with aprotic solvents, resulting in stimuli-responsive materials. Utilization of spectroscopic techniques, statistical analysis, and theoretical methods revealed distinct features corresponding to the relative presence of different species with unique spatial arrangements. Depending on the occupancy of the interlayer space, the subsequent application of dimethyl sulfoxide leads to a swelling of the interlayer space, affecting the orientation and relative distribution of species. Presented study also highlights the importance of in-depth analysis of organic species in confined environments of 2D materials, contributing to the optimization and development of novel applied materials.

Laser modulation of the FePS3 memristors.

Ternary two-dimensional (2D) material-based memristors have garnered significant attention in the fields of machine learning, neuromorphic computing due to their low power consumption, rapid learning, and synaptic-like behavior. Although such memristors often exhibit high ON/OFF ratios and exceptional pulse response characteristics, they have also to face some challenges concerning reusability and switching cycles, which arise from the filament instability issues.. Here we propose a modulation strategy to improve performance of 2D-material memristors with synaptic and flexible features. By laser-modulating few-layer FePS3, we induced the formation of conductive filaments, realized a major improvement in performance of the FePS3 memristors, achieving an on/off ratio of nearly 104, low power consumption at approximately 10-7 W of single switching operation, and maintaining stability even after over 500 cycles. The performance promotion has been ascribed to enhancement of conductive filament induced by laser-modulation. Furthermore, we have identified the effectiveness of our laser modulation under strain by building the high-performance flexible FePS3 memristor. Meanwhile, we discovered a novel strain-dominant erasure method for the flexible memristors. Our work confirms that laser modulation is a viable method for enhancing the performance of 2D material-based memristive devices.&#xD.

Biaxial Strain Transfer in Monolayer MoS2 and WSe2 Transistor Structures.

Monolayer transition metal dichalcogenides are intensely explored as active materials in 2D material-based devices due to their potential to overcome device size limitations, sub-nanometric thickness, and robust mechanical properties. Considering their large band gap sensitivity to mechanical strain, single-layered TMDs are well-suited for strain-engineered devices. While the impact of various types of mechanical strain on the properties of a variety of TMDs has been studied in the past, TMD-based devices have rarely been studied under mechanical deformations, with uniaxial strain being the most common one. Biaxial strain on the other hand, which is an important mode of deformation, remains scarcely studied as far as 2D material devices are concerned. Here, we study the strain transfer efficiency in MoS2- and WSe2-based flexible transistor structures under biaxial deformation. Utilizing Raman spectroscopy, we identify that strains as high as 0.55% can be efficiently and homogeneously transferred from the substrate to the material in the transistor channel. In particular, for the WSe2 transistors, we capture the strain dependence of the higher-order Raman modes and show that they are up to five times more sensitive compared to the first-order ones. Our work demonstrates Raman spectroscopy as a nondestructive probe for strain detection in 2D material-based flexible electronics and deepens our understanding of the strain transfer effects on 2D TMD devices.

Contact Resistance Engineering in WS2-Based FET with MoS2 Under-Contact Interlayer: A Statistical Approach.

One of the primary factors hindering the development of 2D material-based devices is the difficulty of overcoming fabrication processes, which pose a challenge in achieving low-resistance contacts. Widely used metal deposition methods lead to unfavorable Fermi level pinning effect (FLP), which prevents control over the Schottky barrier height at the metal/2D material junction. We propose to harness the FLP effect to lower contact resistance in field-effect transistors (FETs) by using an additional 2D interlayer at the conducting channel and metallic contact interface (under-contact interlayer). To do so, we developed a new approach using the gold-assisted transfer method, which enables the fabrication of heterostructures consisting of TMDs monolayers with complex shapes, prepatterned using e-beam lithography, with lateral dimensions even down to 100 nm. We designed and demonstrated tungsten disulfide (WS2) monolayer-based devices in which the molybdenum disulfide (MoS2) monolayer is placed only in the contact area of the FET, creating an Au/MoS2/WS2 junction, which effectively reduces contact resistance by over 60% and improves the Ion/Ioff ratio 10 times in comparison to WS2-based devices without MoS2 under-contact interlayer. The enhancement in the device operation arises from the FLP effect occurring only at the interface between the metal and the first layer of the MoS2/WS2 heterostructure. This results in favorable band alignment, which enhances the current flow through the junction. To ensure the reproducibility of our devices, we systematically analyzed 160 FET devices fabricated with under-contact interlayer and without it. Statistical analysis shows a consistent improvement in the operation of the device and reveals the impact of contact resistance on key FET performance indicators.

2D Materials in Advanced Electronic Biosensors for Point-of-Care Devices.

Since two-dimensionalal (2D) materials have distinct chemical and physical properties, they are widely used in various sectors of modern technologies. In the domain of diagnostic biodevices, particularly for point-of-care (PoC) biomedical diagnostics, 2D-based field-effect transistor biosensors (bio-FETs) demonstrate substantial potential. Here, in this review article, the operational mechanisms and detection capabilities of biosensing devices utilizing graphene, transition metal dichalcogenides (TMDCs), black phosphorus, and other 2D materials are addressed in detail. The incorporation of these materials into FET-based biosensors offers significant advantages, including low detection limits (LOD), real-time monitoring, label-free diagnosis, and exceptional selectivity. The review also highlights the diverse applications of these biosensors, ranging from conventional to wearable devices, underscoring the versatility of 2D material-based FET devices. Additionally, the review provides a comprehensive assessment of the limitations and challenges faced by these devices, along with insights into future prospects and advancements. Notably, a detailed comparison of FET-based biosensors is tabulated along with various other biosensing platforms and their working mechanisms. Ultimately, this review aims to stimulate further research and innovation in this field while educating the scientific community about the latest advancements in 2D materials-based biosensors.

Anisotropic Fracture of Two-Dimensional Ta2NiSe5.

Anisotropic two-dimensional materials present a diverse range of physical characteristics, making them well-suited for applications in photonics and optoelectronics. While mechanical properties play a crucial role in determining the reliability and efficacy of 2D material-based devices, the fracture behavior of anisotropic 2D crystals remains relatively unexplored. Toward this end, we herein present the first measurement of the anisotropic fracture toughness of 2D Ta2NiSe5 by microelectromechanical system-based tensile tests. Our findings reveal a significant in-plane anisotropic ratio (∼3.0), accounting for crystal orientation-dependent crack paths. As the thickness increases, we observe an intriguing intraplanar-to-interplanar transition of fracture along the a-axis, manifesting as stepwise crack features attributed to interlayer slippage. In contrast, ruptures along the c-axis surprisingly exhibit persistent straightness and smoothness regardless of thickness, owing to the robust interlayer shear resistance. Our work affords a promising avenue for the construction of future electronics based on nanoribbons with atomically sharp edges.

Laser-induced graphene van der Waals contact-enabled high-performance 2D-materials-based field-effect transistor

Establishing robust electrical contact between electrodes and two-dimensional (2D) semiconductors has become an increasingly critical challenge in realizing high-performance 2D material-based devices. This study presents an easy-to-fabricate high-quality van der Waals (vdW) contact strategy, utilizing transferred laser-induced graphene (LIG), for monolayer graphene field-effect transistors (LIG-GFETs). LIG-graphene vdW contacts were formed via a simple transfer and alignment step without any high-temperature or vacuum processes. Excellent electrical properties of LIG-GFETs were achieved, with up to sevenfold enhanced carrier mobilities compared to conventional gold electrode-based GFETs. Experimental investigations and density functional theory simulations elucidated the mechanisms underlying this performance enhancement. Specifically, the superior performance of LIG-GFETs can be attributed to the formation of vdW contacts between the transferred LIG and the monolayer graphene, alongside the doping of the monolayer graphene induced by the O functional groups in the LIG. We also demonstrated that the high performance monolayer MoS2 FETs can be achieved with more than fivefold enhanced carrier mobilities by using LIG vdW contact compared to conventional gold electrode-based MoS2 FETs. This newly developed vdW contact strategy provides new insights into high-performance 2D material-based devices.

Anti-ambipolar transport and logic operation in two-dimensional field-effect transistors using in-series integration of GeAs and SnS2

Germanium arsenide (GeAs) from the IV–V semiconductor family has drawn attention for its anisotropic optical and electrical characteristics as a robust p-type semiconductor with high mobility. Despite its potential, the scope of applications for two-dimensional (2D) GeAs remains limited. In this study, we investigate the in-series integration of GeAs and SnS2 for complementary inverter operation, a crucial element in logic circuits. Moreover, the resulting in-series field-effect transistors reveal a previously undocumented anti-ambipolar behavior in this configuration, with a peak-to-valley ratio exceeding 5000 at a drain-source bias of 2 V. This anti-ambipolar characteristic operates regardless of the direction of current flow, which is rarely seen in conventional anti-ambipolar transistors built with hetero-stacked p–n junctions. Moreover, the in-series structure demonstrates stable operation as a complementary inverter, highlighting the versatile potential of p-type 2D GeAs in diverse optoelectronic applications. This work contributes insights into the transport characteristics of GeAs and its interconnected arrangement with SnS2, offering valuable implications for the development of advanced 2D material-based devices.

Recent Advances in In-Memory Computing: Exploring Memristor and Memtransistor Arrays with 2D Materials.

The conventional computing architecture faces substantial challenges, including high latency and energy consumption between memory and processing units. In response, in-memory computing has emerged as a promising alternative architecture, enabling computing operations within memory arrays to overcome these limitations. Memristive devices have gained significant attention as key components for in-memory computing due to their high-density arrays, rapid response times, and ability to emulate biological synapses. Among these devices, two-dimensional (2D) material-based memristor and memtransistor arrays have emerged as particularly promising candidates for next-generation in-memory computing, thanks to their exceptional performance driven by the unique properties of 2D materials, such as layered structures, mechanical flexibility, and the capability to form heterojunctions. This review delves into the state-of-the-art research on 2D material-based memristive arrays, encompassing critical aspects such as material selection, device performance metrics, array structures, and potential applications. Furthermore, it provides a comprehensive overview of the current challenges and limitations associated with these arrays, along with potential solutions. The primary objective of this review is to serve as a significant milestone in realizing next-generation in-memory computing utilizing 2D materials and bridge the gap from single-device characterization to array-level and system-level implementations of neuromorphic computing, leveraging the potential of 2D material-based memristive devices.

Nanomaterials Based Micro/Nanoelectromechanical System (MEMS and NEMS) Devices.

The micro- and nanoelectromechanical system (MEMS and NEMS) devices based on two-dimensional (2D) materials reveal novel functionalities and higher sensitivity compared to their silicon-base counterparts. Unique properties of 2D materials boost the demand for 2D material-based nanoelectromechanical devices and sensing. During the last decades, using suspended 2D membranes integrated with MEMS and NEMS emerged high-performance sensitivities in mass and gas sensors, accelerometers, pressure sensors, and microphones. Actively sensing minute changes in the surrounding environment is provided by means of MEMS/NEMS sensors, such as sensing in passive modes of small changes in momentum, temperature, and strain. In this review, we discuss the materials preparation methods, electronic, optical, and mechanical properties of 2D materials used in NEMS and MEMS devices, fabrication routes besides device operation principles.

Analysis of p-Type Doping in Graphene Induced by Monolayer-Oxidized TMDs.

Doping is one of the most difficult technological challenges for realizing reliable two-dimensional (2D) material-based semiconductor devices, arising from their ultrathinness. Here, we systematically investigate the impact of different types of nonstoichiometric solid MOx (M are W or Mo) dopants obtained by oxidizing transition metal dichalcogenides (TMDs: WSe2 or MoS2) formed on graphene FETs, which results in p-type doping along with disorders. From the results obtained in this study, we were able to suggest an analytical technique to optimize the optimal UV-ozone (UVO) treatment to achieve high p-type doping concentration in graphene FETs (∼2.5 × 1013 cm-2 in this study) without generating defects, mainly by analyzing the time dependency of D and D' peaks measured by Raman spectroscopy. Furthermore, an analysis of the structure of graphene sheets using TEM indicates that WOx plays a better protective role in graphene, compared to MoOx, suggesting that WOx is more effective for preventing the degradation of graphene during UVO treatment. To enhance the practical application aspect of our work, we have fabricated a graphene photodetector by selectively doping the graphene through oxidized TMDs, creating a p-n junction, which resulted in improved photoresponsivity compared to the intrinsic graphene device. Our results offer a practical guideline for the utilization of surface charge transfer doping of graphene toward CMOS applications.

Potassium hydroxide treatment of layered WSe2 with enhanced electronic performances.

2D WSe2-based electronic devices have received much research interest. However, it is still a challenge to achieve high electronic performance in WSe2-based devices. In this work, we report greatly enhanced performances of different thickness WSe2 ambipolar transistors and demonstrate homogeneous WSe2 inverter devices, which are obtained by using a semiconductor processing-compatible layer removal technique via chemical removal of the surface top WOx layer formed by O2 plasma treatment. Importantly, monolayer WSe2 was realised after several consecutive removal processes, demonstrating that the single layer removal is accurate and reliable. After subsequent removal of the top layer WOx by KOH, the fabricated WSe2 field-effect transistors exhibit greatly enhanced electronic performance along with the high electron and hole mobilities of 40 and 85 cm2 V-1 s-1, respectively. Our work demonstrates that the layer removal technique is an efficient route to fabricate high performance 2D material-based electronic devices.

Temperature dependent charge carrier dynamics in 2D ternary Cu2MoS4 nanoflakes: An effect of electron-phonon coupling.

Two-dimensional transition metal chalcogenides (2D TMCs) like MoS2, WS2 etc., have established significant dominance in the field of nanoscience and nanotechnology, owing to their unique properties like strong light-matter interaction, high carrier mobility, large photo-responsivity etc. Despite the widespread utilization of these binary TMCs, their potential in the advancement of the optoelectronic research is limited due to the constraints in band tuning and charge carrier lifetime. To overcome these limitations, ternary transition metal chalcogenides have emerged as promising alternatives. Although, the optical properties of these materials have never been explored properly. Herein, we have investigated one such promising member of this group, Cu2MoS4 (CMS) using both steady state and time-resolved spectroscopic techniques. The material exhibits a broad range of visible light absorption, peaking at 576nm. Photoluminescence spectroscopy confirmed the presence of both band gap emission and trap state-mediated emissions. Transient absorption spectroscopy unraveled the excited state charge carrier dynamics of CMS in sub-ps timescale, upon irradiation of visible light. We found significant influence of the trap mediated recombination, while Auger process being dominant at high charge density. We extended our study in a wide temperature range (5-300K), which reveals the impact of electron-phonon coupling strength on the band gap and charge carrier dynamics of this material. This detailed study would draw more attention toward the unexplored optical properties of ternary 2D chalcogenides and will open new avenues for the construction of 2D material-based optical devices.

Stamped production of single-crystal hexagonal boron nitride monolayers on various insulating substrates

Controllable growth of two-dimensional (2D) single crystals on insulating substrates is the ultimate pursuit for realizing high-end applications in electronics and optoelectronics. However, for the most typical 2D insulator, hexagonal boron nitride (hBN), the production of a single-crystal monolayer on insulating substrates remains challenging. Here, we propose a methodology to realize the facile production of inch-sized single-crystal hBN monolayers on various insulating substrates by an atomic-scale stamp-like technique. The single-crystal Cu foils grown with hBN films can stick tightly (within 0.35 nm) to the insulating substrate at sub-melting temperature of Cu and extrude the hBN grown on the metallic surface onto the insulating substrate. Single-crystal hBN films can then be obtained by removing the Cu foil similar to the stamp process, regardless of the type or crystallinity of the insulating substrates. Our work will likely promote the manufacturing process of fully single-crystal 2D material-based devices and their applications.

Two-dimensional tellurium-based diodes for RF applications

The research of two-dimensional (2D) Tellurium (Te) or tellurene is thriving to address current challenges in emerging thin-film electronic and optoelectronic devices. However, the study of 2D-Te-based devices for high-frequency applications is still lacking in the literature. This work presents a comprehensive study of two types of radio frequency (RF) diodes based on 2D-Te flakes and exploits their distinct properties in two RF applications. First, a metal-insulator-semiconductor (MIS) structure is employed as a nonlinear device in a passive RF mixer, where the achieved conversion loss at 2.5 GHz and 5 GHz is as low as 24 dB and 29 dB, respectively. Then, a metal-semiconductor (MS) diode is tested as a zero-bias millimeter-wave power detector and reaches an outstanding linear-in-dB dynamic range over 40 dB, while having voltage responsivities as high as 257 V ⋅ W−1 at 1 GHz (up to 1 V detected output voltage) and 47 V ⋅ W−1 at 2.5 GHz (up to 0.26 V detected output voltage). These results show superior performance compared to other 2D material-based devices in a much more mature technological phase. Thus, the authors believe that this work demonstrates the potential of 2D-Te as a promising material for devices in emerging high-frequency electronics.

Thickness-Controlled Synthesis of Uniform Hexagonal Boron Nitride Films on Metal Alloys by Chemical Vapor Deposition

Two-dimensional (2D) multilayer hexagonal boron nitride (hBN) is a superior substrate for other 2D materials due to its insulating property, atomic-scale smoothness, and absence of dangling bonds, enhancing electrical or optical properties in high-performance 2D material-based devices. In most fabrication processes for 2D heterostructure devices, thick hBN flakes exfoliated from bulk have been used because of their high quality and simplicity in the process. However, exfoliated hBN flakes are limited in size and thickness control, impeding scale-up production for industrialization. Therefore, new synthesis strategies are required to overcome the drawback of the exfoliation method. In this work, we investigated the synthesis of large-area, multilayer hBN via atmospheric pressure chemical vapor deposition using single crystalline metal and single crystal alloy substrates. The synthesized results are characterized by optical microscopy, scanning electron microscopy, Raman spectroscopy, atomic force microscopy, etc. These studies provide a more comprehensive understanding of the growth mechanism of hexagonal boron nitride.

Designing high-efficiency electrode contacts to two-dimensional semiconductor Cu2Se

High-efficiency electrode contact plays a pivotal role in achieving 2D material-based high performance nano devices. Recently, monolayer semiconducting Cu2Se with high stability in air and high carrier mobility of about 103 cm2 V−1 s−1 have been experimentally fabricated. Herein, to design high-efficiency electrode contacts for Cu2Se monolayer, the contact properties between Cu2Se monolayer and a series of experimentally fabricated 2D metals (MX2 in T-phase or H-phase, M = Ni, Nb, Ti, V, Co, Zr, and Ta, X = S, Se and Te) are systematically investigated based on first-principles calculations. Considering both Schottky barriers and tunneling barriers of these metal–semiconductor junctions (MSJs), H-NbSe2 is screened out as the most adaptable electrode for monolayer Cu2Se. Moreover, the fermi level pinning effects are discovered in these MSJs due to the potential steps contributed by the interface dipoles. Our work not only provides useful instruction for the design of high-performance 2D nano devices based on Cu2Se monolayer but also offers insights for prospection into the fundamental electronic properties of MSJs.

Imaging Fermi-level hysteresis in nanoscale bubbles of few-layer MoS2

The electrical stability and reliability of two-dimensional (2D) crystal-based devices are mainly determined by charge traps in the device defects. Although nanobubble structures as defect sources in 2D materials strongly affect the device performance, the local charge-trapping behaviors in nanobubbles are poorly understood. Here, we report a Fermi-level hysteresis imaging strategy using Kelvin probe force microscopy to study the origins of charge trapping in nanobubbles of MoS2 on SiO2. We observe that the Fermi-level hysteresis is larger in nanobubbles than in flat regions and increases with the height in a nanobubble, in agreement with our oxide trap band model. We also perform the local transfer curve measurements on the nanobubble structures of MoS2 on SiO2, which exhibit enhanced current-hysteresis windows and reliable programming/erasing operations. Our results provide fundamental knowledge on the local charge-trapping mechanism in nanobubbles, and the capability to directly image hysteresis can be powerful tool for the development of 2D material-based memory devices.

Electronic/Optoelectronic Memory Device Enabled by Tellurium-based 2D van der Waals Heterostructure for in-Sensor Reservoir Computing at the Optical Communication Band.

Although 2D materials are widely explored for data storage and neuromorphic computing, the construction of 2D material-based memory devices with optoelectronic responsivity in the short-wave infrared (SWIR) region for in-sensor reservoir computing (RC) at the optical communication band still remains a big challenge. In this work, an electronic/optoelectronic memory device enabled by tellurium-based 2D van der Waals (vdW) heterostructure is reported, where the ferroelectric CuInP2 S6 and tellurium channel endow this device with both the long-term potentiation/depression by voltage pulses and short-term potentiation by 1550nm laser pulses (a typical wavelength in the conventional fiber optical communication band). Leveraging the rich dynamics, a fully memristive in-sensor RC system that can simultaneously sense, decode, and learn messages transmitted by optical fibers is demonstrated. The reported 2D vdW heterostructure-based memory featuring both the long-term and short-term memory behaviors using electrical and optical pulses in SWIR region has not only complemented the wide spectrum of applications of 2D materials family in electronics/optoelectronics but also paves the way for future smart signal processing systems at the edge.

Upconversion optogenetics-driven biohybrid sensor for infrared sensing and imaging.

Living organisms are far superior to state-of-the-art devices in visual perception as they have evolved a wide number of capabilities that encompass our most advanced technologies. By leveraging the performance of living organisms and directly interfacing them with artificial components, it can use the intricacy and metabolic efficiency of biological visual sensing within artificial machines. Inspired by the molecular basis (transient receptor potential, TRP) for infrared detection of pit-bearing organisms, we propose a TRP-like biohybrid sensor by integrating upconversion nanoparticles (UCNP) and optogenetically engineered cells on a graphene transistor for infrared sensing and imaging. The UCNP converts infrared light irradiation into blue light, the blue light activates the cells expressed with channelrhodopsin-2 (ChR2) and induces transmembrane photocurrent, and the photocurrent is detected by a biocompatible graphene transistor. Stepwise and overall experimental results show that, upon infrared light irradiation, the UCNP can rapidly mediate cellular photocurrents, which further translates into the extra output current of the graphene transistor. More notably, the response speed of the biohybrid sensor is 1∼3 orders of magnitude faster than those of TRPs heterologously expressed in cell lines in the literature, which confirms the response time advantage of the combination of UCNP and ChR2 within the sensor in place of TRPs. The biohybrid sensor can successfully image infrared targets, proving the feasibility of developing bionic infrared sensing devices by biohybrid integration of nonliving nanomaterials and biological components. This work opens up an avenue for biohybrid sensors to develop the bionic infrared vision that promisingly reproduces the functional superiority of natural organisms. STATEMENT OF SIGNIFICANCE: Infrared sensing and imaging have a wide range of military and civilian applications. Organisms have evolved excellent infrared vision with the molecular basis, transient receptor potential (TRP), and the performance is superior to existing state-of-the-art infrared devices. Inspired by this, a TRP-like biohybrid sensor based on upconversion optogenetics and a 2D material-based device is developed for infrared sensing and imaging. The biohybrid sensor has a relatively fast response speed that is 1∼3 orders of magnitude faster than that of the heterologously expressed TRPs, which enables its capability of infrared imaging with a single pixel-based method. This work broadens the spectrum of biohybrid sensing based on engineered cells to infrared, advancing the process of reproducing the excellent infrared detection of organisms.