Reconfigurable Logic‐in‐Memory and Multilingual Artificial Synapses Based on 2D Heterostructures

Nonvolatile logic devices have attracted intensive research attentions recently for energy efficiency computing, where data computing and storage can be realized in the same device structure. Various approaches have been adopted to build such devices; however, the functionality and versatility are still very limited. Here, 2D van der Waals heterostructures based on direct bandgap materials black phosphorus and rhenium disulfide for the nonvolatile ternary logic operations is demonstrated for the first time with the ultrathin oxide layer from the black phosphorus serving as the charge trapping as well as band‐to‐band tunneling layer. Furthermore, an artificial electronic synapse based on this heterostructure is demonstrated to mimic trilingual synaptic response by changing the input base voltage. Besides, artificial neural network simulation based on the electronic synaptic arrays using the handwritten digits data sets demonstrates a high recognition accuracy of 91.3%. This work provides a path toward realizing multifunctional nonvolatile logic‐in‐memory applications based on novel 2D heterostructures.     

Anisotropic Growth of Nonlayered CdS on MoS2 Monolayer for Functional Vertical Heterostructures

2D semiconductors have emerged as a crucial material for use in next‐generation optotelectronics. Similar to microelectronic devices, 2D vertical heterostructures will most likely be the elemental components for future nanoscale electronics and optotelectronics. To date, the components of mostly reported 2D van der Waals heterostructures are restricted to layer crystals. In this work, it is demonstrated that nonlayered semiconductors of CdS can be epitaxially grown on to 2D layered MoS₂ substrate to form a new quasi vertical heterostructure with clean interface by chemical vapor deposition. Photodetectors based on this CdS/MoS₂ heterostructure show broader wavelength response and ≈50‐fold improvement in photoresponsivity, compared to the devices fabricated from MoS₂ monolayer only. This research opens up a way to fabricate a variety of functional quasi heterostructures from nonlayered semiconductors.     

High‐Sensitivity Floating‐Gate Phototransistors Based on WS2 and MoS2

In recent years, 2D layered materials have been considered as promising photon absorption channel media for next‐generation phototransistors due to their atomic thickness, easily tailored single‐crystal van der Waals heterostructures, ultrafast optoelectronic characteristics, and broadband photon absorption. However, the photosensitivity obtained from such devices, even under a large bias voltage, is still unsatisfactory until now. In this paper, high‐sensitivity phototransistors based on WS₂ and MoS₂ are proposed, designed, and fabricated with gold nanoparticles (AuNPs) embedded in the gate dielectric. These AuNPs, located between the tunneling and blocking dielectric, are found to enable efficient electron trapping in order to strongly suppress dark current. Ultralow dark current (10^?11 A), high photoresponsivity (1090 A W^?1), and high detectivity (3.5 × 10¹¹ Jones) are obtained for the WS₂ devices under a low source/drain and a zero gate voltage at a wavelength of 520 nm. These results demonstrate that the floating‐gate memory structure is an effective configuration to achieve high‐performance 2D electronic/optoelectronic devices.     

Step-By-Step Atomic Insights into Structural Reordering from 2D to 3D MoS2

Vertically stacked low-dimensional heterostructures are outstanding systems both for exploring fundamental physics and creating new devices. Due to nanometer-scale building blocks, atomic scale phenomena become for them of fundamental importance, including during device operation. These can be accessed in situ in aberration-corrected scanning transmission electron microscopy (STEM) experiments. Here, the dynamics of a graphene-MoS₂ heterostructure are studied under Joule heating, where the graphene serves as a high temperature atomically thin and electron transparent “hot plate” for the MoS₂. Structural dynamics and evolution of the system are shown at the atomic scale, demonstrating that at the highest temperatures (estimated to exceed 2000 K), the continuous 2D MoS₂ transforms into separated 3D nanocrystals, initiated by sulfur vacancy creation and migration followed by formation of voids and clustering at their edges. The resulting nanocrystals exhibit predominantly hexagonal shapes with the 2H and hybrid (2H/3R, 3R/TZ) polytypes. The observed morphology of the crystals is further discussed during and after the transformation, as well as their different edge configurations and stability under electron irradiation. These observations of MoS₂ at extreme temperatures provide insights into the operation of devices based on graphene/MoS₂ heterostructures and ultimately may help device fabrication techniques to create MoS₂-based nanostructures, for example, in hydrogen evolution reaction applications.     

Interfacial Charge Behavior Modulation in Perovskite Quantum Dot‐Monolayer MoS2 0D‐2D Mixed‐Dimensional van der Waals Heterostructures

Fundamental understanding of charge behavior inside heterostructures is of vital importance for advancing high‐performance optoelectronic applications. However, the charge behavior of 0D‐2D mixed‐dimensional van der Waals heterostructures (MvdWHs) in the photoexcited state remains elusive. In this work, an energy band alignment protocol is adopted to realize effective energy band structure engineering inside 0D‐2D MvdWHs of perovskite quantum dots and MoS₂ monolayer with precisely designed typical type I and type II heterostructures, respectively. A profile and in‐depth understanding of interfacial photoinduced charge behavior is determined from two opposite perspectives based on MvdWHs. Sufficient comparison of a series of optical characterization results, including Raman shift, quenched photoluminescence, visualized suppressed fluorescence intensity, and shortened fluorescence lifetime imaging, clearly verifies that interfacial charge behavior can be tailored by varying the band alignment in 0D‐2D MvdWHs. Furthermore, the photoresponse performance and the relatively stronger and weaker photogating effects of such MvdWH‐based phototransistors also demonstrate modulation of interfacial charge behavior in 0D‐2D MvdWHs via energy band structure engineering, which is still feasible for optoelectronic performance optimization. These results are expected to shed light on designing novel functional devices and advancing the development process of 0D‐2D MvdWHs in the foreseeable future.     

Polarization-Resolved Broadband MoS2/Black Phosphorus/MoS2 Optoelectronic Memory with Ultralong Retention Time and Ultrahigh Switching Ratio

The rapidly emerging requirement for device miniaturization and structural flexibility make 2D semiconductors and their van der Waals (vdWs) heterostructures extremely attractive for nonvolatile optoelectronic memory (NOM) applications. Although several concepts for 2D NOM have been demonstrated, multi-heterojunction devices capable of further improving storage performance have received little attention. This work reports a concept for MoS₂/black phosphorus (BP)/MoS₂ multi-heterojunction NOM with artificial trap sites through the BP oxidation, in which the trapped holes at BP/PO_x interface intrigue a persistent photoconductivity that hardly recovers within the experimental time scales (exceeding 10⁴ s). As a result of the interfacial trap-controlled charge injection, the device exhibits excellent photoresponsive memory characteristics, including a record high detectivity of ≈1.2 × 10¹⁶ Jones, a large light-to-dark switching ratio of ≈1.5 × 10⁷_, an ultralow off-state current of ≈1.2 pA, and an outstanding multi-bit storage capacity (11 storage states, 546 nC state^–1). In addition, the middle BP layer in the multi-heterojunction enables broadband spectrum distinction (375–1064 nm), together with a high polarization ratio of 8.4. The obtained results represent the significant step toward the high-density integration of optoelectronic memories with 2D vdWs heterostructures.     

Novel and Enhanced Optoelectronic Performances of Multilayer MoS2–WS2 Heterostructure Transistors

Van der Waals heterostructures designed by assembling isolated two‐dimensional (2D) crystals have emerged as a new class of artificial materials with interesting and unusual physical properties. Here, the multilayer MoS₂–WS₂ heterostructures with different configurations are reported and their optoelectronic properties are studied. It is shown that the new heterostructured material possesses new functionalities and superior electrical and optoelectronic properties that far exceed the one for their constituents, MoS₂ or WS₂. The vertical transistor exhibits a novel rectifying and bipolar behavior, and can also act as photovoltaic cell and self‐driven photodetector with photo‐switching ratio exceeding 10³. The planar device also exhibits high field‐effect ON/OFF ratio (>10⁵), high electron mobility of 65 cm²/Vs, and high photo­responsivity of 1.42 A/W compared to that in isolated multilayer MoS₂ or WS₂ nanoflake transistors. The results suggest that formation of MoS₂–WS₂ heterostructures could significantly enhance the performance of optoelectronic devices, thus open up possibilities for future nanoelectronic, photovoltaic, and optoelectronic applications.     

Self‐Aligned and Scalable Growth of Monolayer WSe2–MoS2 Lateral Heterojunctions

2D layered heterostructures have attracted intensive interests due to their unique optical, transport, and interfacial properties. The laterally stitched heterojunction based on dissimilar 2D transition metal dichalcogenides forms an intrinsic p–n junction without the necessity of applying an external voltage. However, no scalable processes are reported to construct the devices with such lateral heterostructures. Here, a scalable strategy, two‐step and location‐selective chemical vapor deposition, is reported to synthesize self‐aligned WSe₂–MoS₂ monolayer lateral heterojunction arrays and demonstrates their light‐emitting devices. The proposed fabrication process enables the growth of high‐quality interfaces and the first successful observation of electroluminescence at the WSe₂–MoS₂ lateral heterojunction. The electroluminescence study has confirmed the type‐I alignment at the interface rather than commonly believed type‐II alignment. This self‐aligned growth process paves the way for constructing various 2D lateral heterostructures in a scalable manner, practically important for integrated 2D circuit applications.     

Phototransistors with Negative or Ambipolar Photoresponse Based on As‐Grown Heterostructures of Single‐Walled Carbon Nanotube and MoS2

A facile synthesis method for the heterostructures of single‐walled carbon nanotubes (SWCNTs) and few‐layer MoS₂ is reported. The heterostructures are realized by in situ chemical vapor deposition of MoS₂ on individual SWCNTs. Field effect transistors based on the heterostructures display different transfer characteristics depending on the formation of MoS₂ conduction channels along SWCNTs. Under light illumination, negative photoresponse originating from charge transfer from MoS₂ to SWCNT is observed while positive photoresponse is observed in MoS₂ conduction channels, leading to ambipolar photoresponse in devices with both SWCNT and MoS₂ channels. The heterostructure phototransistor, for negative photoresponse, exhibits high responsivity (100–1000 AW^?1) at low bias voltages (0.1 V) in the visible spectrum (500–700 nm) by combining high mobility conduction channel (SWCNT) with efficient light absorber (MoS₂).     

Low‐Power Nonvolatile Charge Storage Memory Based on MoS2 and an Ultrathin Polymer Tunneling Dielectric

Low‐power, nonvolatile memory is an essential electronic component to store and process the unprecedented data flood arising from the oncoming Internet of Things era. Molybdenum disulfide (MoS₂) is a 2D material that is increasingly regarded as a promising semiconductor material in electronic device applications because of its unique physical characteristics. However, dielectric formation of an ultrathin low‐k tunneling on the dangling bond‐free surface of MoS₂ is a challenging task. Here, MoS₂‐based low‐power nonvolatile charge storage memory devices are reported with a poly(1,3,5‐trimethyl‐1,3,5‐trivinyl cyclotrisiloxane) (pV3D3) tunneling dielectric layer formed via a solvent‐free initiated chemical vapor deposition (iCVD) process. The surface‐growing polymerization and low‐temperature nature of the iCVD process enable the conformal growing of low‐k (≈2.2) pV3D3 insulating films on MoS₂. The fabricated memory devices exhibit a tunable memory window with high on/off ratio (≈10⁶), excellent retention times of 10⁵ s with an extrapolated time of possibly years, and an excellent cycling endurance of more than 10³ cycles, which are much higher than those reported previously for MoS₂‐based memory devices. By leveraging the inherent flexibility of both MoS₂ and polymer dielectric films, this research presents an important milestone in the development of low‐power flexible nonvolatile memory devices.     

2D TMD Channel Transistors with ZnO Nanowire Gate for Extended Nonvolatile Memory Applications

2D transition metal dichalcogenides (TMDs) have been extensively studied due to their excellent physical properties. Mixed dimensional devices including 2D materials have also been studied, motivated by the possibility of any synergy effect from unique structures. However, only few such studies have been conducted. Here, semiconducting 1D ZnO nanowires are used as thin gate material to support 2D TMD field effect transistors (FETs) and 2D stack‐based interface trap nonvolatile memory. For the trap memory, deep level electron traps formed at the first MoS₂/second MoS₂ stack interface are exploited, since the first MoS₂ is treated in an atomic layer deposition chamber for a short while. On the one hand, a complementary inverter type memory device can also be achieved using a long single ZnO wire as a common gate to simultaneously support both n‐ and p‐channel TMD FETs. In addition, it is found that the semiconducting ZnO nanowire itself operates as an n‐type channel when the TMD materials can become a top‐gate to charge the ZnO channel. It means that 2D (bottom gated) and 1D channel (top gated) FETs are respectively operational in a single device structure. The 1D–2D mixed devices seem deserving broad attention in both aspects of novelty and functionality.     

Nonvolatile Charge Injection Memory Based on Black Phosphorous 2D Nanosheets for Charge Trapping and Active Channel Layers

2D van der Waals atomic crystal materials have great potential for use in future nanoscale electronic and optoelectronic applications owing to their unique properties such as a tunable energy band gap according to their thickness or number of layers. Recently, black phosphorous (BP) has attracted significant interest because it is a single‐component material like graphene and has high mobility, a direct band gap, and exhibits ambipolar transition behavior. This study reports on a charge injection memory field‐effect transistor on a glass substrate, where few‐layer BPs act as the active channel and charge trapping layers, and Al₂O₃ films grown by atomic layer deposition act as the tunneling and blocking layers. Because of the ambipolar properties of BP nanosheets, both electrons and holes are involved in the charge trapping process, resulting in bilateral threshold voltage shifts with a large memory window of 22 V. Finally, a memory circuit of a resistive‐load inverter is implemented that converts analog signals (current) to digital signals (voltage). Such a memory inverter also shows a clear memory window and distinct memory on/off switching characteristics.     

Van der Waals p–n Junction Based on an Organic–Inorganic Heterostructure

Organic–inorganic heterostructures are an emerging topic that is very interesting for optoelectronics. Here, non‐conventional p–n junctions are investigated using organic rubrene single crystal and 2D MoS₂ as the p‐ and n‐type semiconducting materials, respectively. The current‐rectifying behavior is clearly observed in the junction device. The rectification ratio can be electrically tuned by the gate voltage due to the 2D nature of the heterostructure. The devices also show good photoresponse properties with a photoresponsivity of ≈500 mA W^?1 and a fast response time. These findings suggest a new route to facilitate the design of nanoelectronic and optoelectronic devices based on layered inorganics and organics.     

2D Metal–Organic Framework Nanosheets with Time‐Dependent and Multilevel Memristive Switching

Metal–organic framework (MOF) nanosheets have attracted significant interests for sensing, electrochemical, and catalytic applications. Most significantly, 2D MOF with highly accessible sites on the surface is expected to be applicable in data storage. Here, the memory device is first demonstrated by employing M‐TCPP (TCPP: tetrakis(4‐carboxyphenyl)porphyrin, M: metal) as resistive switching (RS) layer. The as‐fabricated resistive random access memory (RRAM) devices exhibit a typical electroforming free bipolar switching characteristic with on/off ratio of 10³, superior retention, and reliability performance. Furthermore, the time‐dependent RS behaviors under constant voltage stress of 2D M‐TCPP–based RRAMs are systematically investigated. The properties of the percolated conducting paths are revealed by the Weibull distribution by collecting the measured turn‐on time. The multilevel information storage state can be gotten by setting a series of compliance current. The charge trapping assisted hopping is proposed as operation principle of the MOF‐based RRAMs which is further confirmed by atomic force microscopy at electrical modes. The research is highly relevant for practical operation of 2D MOF nanosheet–based RRAM, since the time widths, magnitudes of pulses, and multilevel‐data storage can be potentially set.     

Gas Sensing of NiO‐SCCNT Core–Shell Heterostructures: Optimization by Radial Modulation of the Hole‐Accumulation Layer

Hierarchical core–shell (C–S) heterostructures composed of a NiO shell deposited onto stacked‐cup carbon nanotubes (SCCNTs) are synthesized by atomic layer deposition (ALD). A film of NiO particles (0.80–21.8 nm in thickness) is uniformly deposited onto the inner and outer walls of the SCCNTs. The electrical resistance of the samples is found to increase of many orders of magnitude with the increasing of the NiO thickness. The response of NiO–SCCNT sensors toward low concentrations of acetone and ethanol at 200 °C is studied. The sensing mechanism is based on the modulation of the hole‐accumulation region in the NiO shell layer upon chemisorption of the reducing gas molecules. The electrical conduction mechanism is further studied by the incorporation of an Al₂O₃ dielectric layer at NiO and SCCNT interfaces. The investigations on NiO–Al₂O₃–SCCNT, Al₂O₃–SCCNT, and NiO–SCCNT coaxial heterostructures reveal that the sensing mechanism is strictly related to the NiO shell layer. The remarkable performance of the NiO–SCCNT sensors toward acetone and ethanol benefits from the conformal coating by ALD, large surface area of the SCCNTs, and the optimized p‐NiO shell layer thickness followed by the radial modulation of the space‐charge region.     

Patterned Growth of P‐Type MoS2 Atomic Layers Using Sol–Gel as Precursor

2D layered MoS₂ has drawn intense attention for its applications in flexible electronic, optoelectronic, and spintronic devices. Most of the MoS₂ atomic layers grown by conventional chemical vapor deposition techniques are n‐type due to the abundant sulfur vacancies. Facile production of MoS₂ atomic layers with p‐type behavior, however, remains challenging. Here, a novel one‐step growth has been developed to attain p‐type MoS₂ layers in large scale by using Mo‐containing sol–gel, including 1% tungsten (W). Atomic‐resolution electron microscopy characterization reveals that small tungsten oxide clusters are commonly present on the as‐grown MoS₂ film due to the incomplete reduction of W precursor at the reaction temperature. These omnipresent small tungsten oxide clusters contribute to the p‐type behavior, as verified by density functional theory calculations, while preserving the crystallinity of the MoS₂ atomic layers. The Mo containing sol–gel precursor is compatible with the soft‐lithography techniques, which enables patterned growth of p‐type MoS₂ atomic layers into regular arrays with different shapes, holding great promise for highly integrated device applications. Furthermore, an atomically thin p–n junction is fabricated by the as‐prepared MoS₂, which shows strong rectifying behavior.     

0D/2D Heterostructures Vertical Single Electron Transistor

Mixed-dimensional heterostructures formed by the stacking of 2D materials with nanostructures of distinct dimensionality constitute a new class of nanomaterials that offers multifunctionality that goes beyond those of single dimensional systems. An unexplored architecture of single electron transistor (SET) is developed that employs heterostructures made of nanoclusters (0D) grown on a 2D molybdenum disulfide (MoS₂) channel. Combining the large Coulomb energy of the nanoclusters with the electronic capabilities of the 2D layer, the concept of 0D–2D vertical SET is unveiled. The MoS₂ underneath serves both as a charge tunable channel interconnecting the electrode, and as bottom electrode for each v-SET cell. In addition, its atomic thickness makes it thinner than the Debye screening length, providing electric field transparency functionality that allows for an efficient electric back gate control of the nanoclusters charge state. The Coulomb diamond pattern characteristics of SET are reported, with specific doping dependent nonlinear features arising from the 0D/2D geometry that are elucidated by theoretical modeling. These results hold promise for multifunctional single electron device taking advantage of the versatility of the 2D materials library, with as example envisioned spintronics applications while coupling quantum dots to magnetic 2D material, or to ferroelectric layers for neuromorphic devices.     

Low‐Temperature‐Grown Transition Metal Oxide Based Storage Materials and Oxide Transistors for High‐Density Non‐volatile Memory

An effective stacked memory concept utilizing all‐oxide‐based device components for future high‐density nonvolatile stacked structure data storage is developed. GaInZnO (GIZO) thin‐film transistors, grown at room temperature, are integrated with one‐diode (CuO/InZnO)–one‐resistor (NiO) (1D–1R) structure oxide storage node elements, fabricated at room temperature. The low growth temperatures and fabrication methods introduced in this paper allow the demonstration of a stackable memory array as well as integrated device characteristics. Benefits provided by low‐temperature processes are demonstrated by fabrication of working devices over glass substrates. Here, the device characteristics of each individual component as well as the characteristics of a combined select transistor with a 1D–1R cell are reported. X‐ray photoelectron spectroscopy analysis of a NiO resistance layer deposited by sputter and atomic layer deposition confirms the importance of metallic Ni content in NiO for bi‐stable resistance switching. The GIZO transistor shows a field‐effect mobility of 30 cm² V⁻¹ s⁻¹, a V_th of +1.2 V, and a drain current on/off ratio of up to 10⁸, while the CuO/InZnO heterojunction oxide diode has forward current densities of 2 × 10⁴ A cm⁻². Both of these materials show the performance of state‐of‐the‐art oxide devices.     

Ultraviolet‐Light‐Induced Reversible and Stable Carrier Modulation in MoS2 Field‐Effect Transistors

The tuning of charge carrier concentrations in semiconductor is necessary in order to approach high performance of the electronic and optoelectronic devices. It is demonstrated that the charge‐carrier density of single‐layer (SL), bilayer (BL), and few‐layer (FL) MoS₂ nanosheets can be finely and reversibly tuned with N₂ and O₂ gas in the presence of deep‐ultraviolet (DUV) light. After exposure to N₂ gas in the presence of DUV light, the threshold voltages of SL, BL, and FL MoS₂ field‐effect transistors (FETs) shift towards negative gate voltages. The exposure to N₂ gas in the presence of DUV light notably improves the drain‐to‐source current, carrier density, and charge‐carrier mobility for SL, BL, and FL MoS₂ FETs. Subsequently, the same devices are exposed to O₂ gas in the presence of DUV light for different periods and the electrical characteristics are completely recovered after a certain time. The doping by using the combination of N₂ and O₂ gas with DUV light provides a stable, effective, and facile approach for improving the performance of MoS₂ electronic devices.     

Mixed‐Dimensional 1D ZnO–2D WSe2 van der Waals Heterojunction Device for Photosensors

2D layered van der Waals (vdW) atomic crystals are an emerging class of new materials that are receiving increasing attention owing to their unique properties. In particular, the dangling‐bond‐free surface of 2D materials enables integration of differently dimensioned materials into mixed‐dimensional vdW heterostructures. Such mixed‐dimensional heterostructures herald new opportunities for conducting fundamental nanoscience studies and developing nanoscale electronic/optoelectronic applications. This study presents a 1D ZnO nanowire (n‐type)–2D WSe₂ nanosheet (p‐type) vdW heterojunction diode for photodetection and imaging process. After amorphous fluoropolymer passivation, the ZnO–WSe₂ diode shows superior performance with a much‐enhanced rectification (ON/OFF) ratio of over 10⁶ and an ideality factor of 3.4–3.6 due to the carbon–fluorine (C? F) dipole effect. This heterojunction device exhibits spectral photoresponses from ultraviolet (400 nm) to near infrared (950 nm). Furthermore, a prototype visible imager is demonstrated using the ZnO–WSe₂ heterojunction diode as an imaging pixel. To the best of our knowledge, this is the first demonstration of an optoelectronic device based on a 1D–2D hybrid vdW heterojunction. This approach using a 1D ZnO–2D WSe₂ heterojunction paves the way for the further development of electronic/optoelectronic applications using mixed‐dimensional vdW heterostructures.