Eight In. Wafer-Scale Epitaxial Monolayer MoS2.

Large-scale, high-quality, and uniform monolayer molybdenum disulfide (MoS2) films are crucial for their applications in next-generation electronics and optoelectronics. Epitaxy is a mainstream technique for achieving high-quality MoS2 films and is demonstrated at a wafer scale up to 4-in. In this study, the epitaxial growth of 8-in. wafer-scale highly oriented monolayer MoS2 on sapphire is reported as with excellent spatial homogeneity, using a specially designed vertical chemical vapor deposition (VCVD) system. Field effect transistors (FETs) based on the as-grown 8-in. wafer-scale monolayer MoS2 film are fabricated and exhibit high performances, with an average mobility and an on/off ratio of 53.5 cm2 V-1 s-1 and 107, respectively. In addition, batch fabrication of logic devices and 11-stage ring oscillators are also demonstrated, showcasing excellent electrical functions. This work may pave the way of MoS2 in practical industry-scale applications.

Epitaxy of wafer-scale single-crystal MoS2 monolayer via buffer layer control.

Monolayer molybdenum disulfide (MoS2), an emergent two-dimensional (2D) semiconductor, holds great promise for transcending the fundamental limits of silicon electronics and continue the downscaling of field-effect transistors. To realize its full potential and high-end applications, controlled synthesis of wafer-scale monolayer MoS2 single crystals on general commercial substrates is highly desired yet challenging. Here, we demonstrate the successful epitaxial growth of 2-inch single-crystal MoS2 monolayers on industry-compatible substrates of c-plane sapphire by engineering the formation of a specific interfacial reconstructed layer through the S/MoO3 precursor ratio control. The unidirectional alignment and seamless stitching of MoS2 domains across the entire wafer are demonstrated through cross-dimensional characterizations ranging from atomic- to centimeter-scale. The epitaxial monolayer MoS2 single crystal shows good wafer-scale uniformity and state-of-the-art quality, as evidenced from the ~100% phonon circular dichroism, exciton valley polarization of ~70%, room-temperature mobility of ~140 cm2v-1s-1, and on/off ratio of ~109. Our work provides a simple strategy to produce wafer-scale single-crystal 2D semiconductors on commercial insulator substrates, paving the way towards the further extension of Moore's law and industrial applications of 2D electronic circuits.

Scaling of MoS2 Transistors and Inverters to Sub-10 nm Channel Length with High Performance.

Two-dimensional (2D) semiconductors such as monolayer molybdenum disulfide (MoS2) are promising building blocks for ultrascaled field effect transistors (FETs), benefiting from their atomic thickness, dangling-bond-free flat surface, and excellent gate controllability. However, despite great prospects, the fabrication of 2D ultrashort channel FETs with high performance and uniformity remains a challenge. Here, we report a self-encapsulated heterostructure undercut technique for the fabrication of sub-10 nm channel length MoS2 FETs. The fabricated 9 nm channel MoS2 FETs exhibit superior performances compared with sub-15 nm channel length including the competitive on-state current density of 734/433 µA/µm at VDS = 2/1 V, record-low DIBL of ∼50 mV/V, and superior on/off ratio of 3 × 107 and low subthreshold swing of ∼100 mV/dec. Furthermore, the ultrashort channel MoS2 FETs fabricated by this new technique show excellent homogeneity. Thanks to this, we scale the monolayer inverter down to sub-10 nm channel length.

2D Semiconductor Based Flexible Photoresponsive Ring Oscillators for Artificial Vision Pixels.

Artificial retina implantation provides an effective and feasible attempt for vision recovery in addition to retinal transplantation. The most advanced artificial retinas ever developed based on silicon technology are rigid and thus less compatible with the biosystem. Here we demonstrate flexible photoresponsive ring oscillators (PROs) based on the 2D semiconductor MoS2 for artificial retinas. Under natural light illuminations, arrayed PROs on flexible substrates serving as vision pixels can efficiently output light-intensity-dependent electrical pulses that are processable and transmittable in the human visual nerve system. Such PROs can work under low supply voltages below 1 V with a record-low power consumption, e.g. only 12.4 nW at a light intensity of 10 mW/cm2, decreased by ∼500 times compared with that of the state-of-the-art silicon devices. Such flexible artificial retinas with a simple device structure, high light-to-signal conversion efficiency, ultralow power consumption, and high tunability provide an alternative prosthesis for further clinical trials.

Curvature-Induced One-Dimensional Phonon Polaritons at Edges of Folded Boron Nitride Sheets.

Generation and manipulation of phonon polaritons are of paramount importance for understanding the interaction between an electromagnetic field and dielectric materials and furthering their application in mid-infrared optical communication. However, the formation of tunable one-dimensional phonon polaritons has been rarely realized in van der Waals layered structures. Here we report the discovery of curvature-induced phonon polaritons localized at the crease of folded hexagonal boron nitrides (h-BNs) with a few atomic layers using monochromated electron energy-loss spectroscopy. Compared to bulk regions, the creased-localized signals undergo an abnormal blue-shift of 1.4 meV. First-principles calculations reveal that the energy shift arises from the optical phonon hardening in the curled region. Interestingly, the curvature-induced phonon polariton can also be controllably achieved via an electron-beam etching approach. This work opens an avenue of tailoring local electromagnetic response and creating unique phonon polariton modes in van der Waals layered materials for diverse applications.

Imaging gate-tunable Tomonaga-Luttinger liquids in 1H-MoSe2 mirror twin boundaries.

One-dimensional electron systems exhibit fundamentally different properties than higher-dimensional systems. For example, electron-electron interactions in one-dimensional electron systems have been predicted to induce Tomonaga-Luttinger liquid behaviour. Naturally occurring grain boundaries in single-layer transition metal dichalcogenides exhibit one-dimensional conducting channels that have been proposed to host Tomonaga-Luttinger liquids, but charge density wave physics has also been suggested to explain their behaviour. Clear identification of the electronic ground state of this system has been hampered by an inability to electrostatically gate such boundaries and tune their charge carrier concentration. Here we present a scanning tunnelling microscopy and spectroscopy study of gate-tunable mirror twin boundaries in single-layer 1H-MoSe2 devices. Gating enables scanning tunnelling microscopy and spectroscopy for different mirror twin boundary electron densities, thus allowing precise characterization of electron-electron interaction effects. Visualization of the resulting mirror twin boundary electronic structure allows unambiguous identification of collective density wave excitations having two velocities, in quantitative agreement with the spin-charge separation predicted by finite-length Tomonaga-Luttinger liquid theory.

UItra-low friction and edge-pinning effect in large-lattice-mismatch van der Waals heterostructures.

Two-dimensional heterostructures are excellent platforms to realize twist-angle-independent ultra-low friction due to their weak interlayer van der Waals interactions and natural lattice mismatch. However, for finite-size interfaces, the effect of domain edges on the friction process remains unclear. Here we report the superlubricity phenomenon and the edge-pinning effect at MoS2/graphite and MoS2/hexagonal boron nitride van der Waals heterostructure interfaces. We found that the friction coefficients of these heterostructures are below 10-6. Molecular dynamics simulations corroborate the experiments, which highlights the contribution of edges and interface steps to friction forces. Our experiments and simulations provide more information on the sliding mechanism of finite low-dimensional structures, which is vital to understand the friction process of laminar solid lubricants.

Ultrahigh-resolution scanning microwave impedance microscopy of moiré lattices and superstructures.

Two-dimensional heterostructures composed of layers with slightly different lattice vectors exhibit new periodic structure known as moiré lattices, which, in turn, can support novel correlated and topological phenomena. Moreover, moiré superstructures can emerge from multiple misaligned moiré lattices or inhomogeneous strain distributions, offering additional degrees of freedom in tailoring electronic structure. High-resolution imaging of the moiré lattices and superstructures is critical for understanding the emerging physics. Here, we report the imaging of moiré lattices and superstructures in graphene-based samples under ambient conditions using an ultrahigh-resolution implementation of scanning microwave impedance microscopy. Although the probe tip has a gross radius of ~100 nm, spatial resolution better than 5 nm is achieved, which allows direct visualization of the structural details in moiré lattices and the composite super-moiré. We also demonstrate artificial synthesis of novel superstructures, including the Kagome moiré arising from the interplay between different layers.

Artificial Synapse Based on van der Waals Heterostructures with Tunable Synaptic Functions for Neuromorphic Computing.

Two-dimensional (2D) materials and van der Waals heterostructures have attracted tremendous attention because of their appealing electronic, mechanical, and optoelectronic properties, which offer the possibility to extend the range of functionalities for diverse potential applications. Here, we fabricate a novel multiterminal device with dual-gate based on 2D material van der Waals heterostructures. Such a multiterminal device exhibited excellent nonvolatile multilevel resistance switching performance controlled by the source-drain voltage and back-gate voltage. Based on these features, heterosynaptic plasticity, in which the synaptic weight can be tuned by another modulatory interneuron, has been mimicked. A tunable analogue weight update (both on/off ratio and update nonlinearity) of synapse with high speed (50 ns) and low energy (∼7.3 fJ) programming has been achieved. These results demonstrate the great potential of the artificial synapse based on van der Waals heterostructures for neuromorphic computing.

Static and Dynamic Piezopotential Modulation in Piezo-Electret Gated MoS2 Field-Effect Transistor.

The piezotronic effect links the mechanical stimuli with various semiconductor devices, promising for low-power-consuming electronic devices, sensitive sensors, and interactive control systems. The persistent requirement for external strains in piezotronic modulation may hinder its application in some circumstances (such as devices on rigid substrate or complicated synergistic piezoelectric modulation on multidevice). Here, we propose an efficient method to realize piezoelectric modulation of optical and electrical properties of MoS2 FET in both static and dynamic manner, expanding the application of piezotronics. Through capacitive coupling between piezo-electret and MoS2 FET, the remanent piezo-potential can efficiently tune the Fermi level of MoS2, programming the initial electrical property for subsequent fabrication of sophisticated devices. The external strain can induce enhanced piezo-potentials to further affect the energy band bending of MoS2 channel, giving rise to high-performance strain sensors (large gauge factor ∼4800, fast response time ∼0.15 s, and good durability >1000 s). The proposed static and dynamic piezopotential tuned MoS2 FET is easy to extend to devices based on other materials, which is highly desired in tunable sensory systems, active flexible electronics, and human-machine interface.

Tuning Charge Transport in Aromatic-Ring Single-Molecule Junctions via Ionic-Liquid Gating.

Achieving gate control with atomic precision, which is crucial to the transistor performance on the smallest scale, remains a challenge. Herein we report a new class of aromatic-ring molecular nanotransistors based on graphene-molecule-graphene single-molecule junctions by using an ionic-liquid gate. Experimental phenomena and theoretical calculations confirm that this ionic-liquid gate can effectively modulate the alignment between molecular frontier orbitals and the Fermi energy level of graphene electrodes, thus tuning the charge-transport properties of the junctions. In addition, with a small gate voltage (|VG |≤1.5 V) ambipolar charge transport in electrochemically inactive molecular systems (EG >3.5 eV) is realized. These results offer a useful way to build high-performance single-molecule transistors, thus promoting the prospects for molecularly engineered electronic devices.

Magnetotransport Properties of Graphene Nanoribbons with Zigzag Edges.

The determination of the electronic structure by edge geometry is unique to graphene. In theory, an evanescent nonchiral edge state is predicted at the zigzag edges of graphene. Up to now, the approach used to study zigzag-edged graphene has mostly been limited to scanning tunneling microscopy. The transport properties have not been revealed. Recent advances in hydrogen plasma-assisted "top-down" fabrication of zigzag-edged graphene nanoribbons (Z-GNRs) have allowed us to investigate edge-related transport properties. In this Letter, we report the magnetotransport properties of Z-GNRs down to ∼70 nm wide on an h-BN substrate. In the quantum Hall effect regime, a prominent conductance peak is observed at Landau ν=0, which is absent in GNRs with nonzigzag edges. The conductance peak persists under perpendicular magnetic fields and low temperatures. At a zero magnetic field, a nonlocal voltage signal, evidenced by edge conduction, is detected. These prominent transport features are closely related to the observable density of states at the hydrogen-etched zigzag edge of graphene probed by scanning tunneling spectroscopy, which qualitatively matches the theoretically predicted electronic structure for zigzag-edged graphene. Our study gives important insights for the design of new edge-related electronic devices.

Emergence of Interfacial Polarons from Electron-Phonon Coupling in Graphene/h-BN van der Waals Heterostructures.

van der Waals heterostructures, vertical stacks of layered materials, offer new opportunities for novel quantum phenomena which are absent in their constituent components. Here we report the emergence of polaron quasiparticles at the interface of graphene/hexagonal boron nitride (h-BN) heterostructures. Using nanospot angle-resolved photoemission spectroscopy, we observe zone-corner replicas of h-BN valence band maxima, with energy spacing coincident with the highest phonon energy of the heterostructure, an indication of Fröhlich polaron formation due to forward-scattering electron-phonon coupling. Parabolic fitting of the h-BN bands yields an effective mass enhancement of ∼2.3, suggesting an intermediate coupling strength. Our theoretical simulations based on Migdal-Eliashberg theory corroborate the experimental results, allowing the extraction of microscopic physical parameters. Moreover, renormalization of graphene π-band is observed due to the hybridization with the h-BN band. Our work generalizes the polaron study from transition metal oxides to van der Waals heterostructures with higher material flexibility, highlighting interlayer coupling as an extra degree of freedom to explore emergent phenomena.

Graphene-Contacted Ultrashort Channel Monolayer MoS2 Transistors.

2D semiconductors are promising channel materials for field-effect transistors (FETs) with potentially strong immunity to short-channel effects (SCEs). In this paper, a grain boundary widening technique is developed to fabricate graphene electrodes for contacting monolayer MoS2 . FETs with channel lengths scaling down to ≈4 nm can be realized reliably. These graphene-contacted ultrashort channel MoS2 FETs exhibit superior performances including the nearly Ohmic contacts and excellent immunity to SCEs. This work provides a facile route toward the fabrication of various 2D material-based devices for ultrascaled electronics.

Highly Sensitive MoS2 Humidity Sensors Array for Noncontact Sensation.

Recently, 2D materials exhibit great potential for humidity sensing applications due to the fact that almost all atoms are at the surface. Therefore, the quality of the material surface becomes the key point for sensitive perception. This study reports an integrated, highly sensitive humidity sensors array based on large-area, uniform single-layer molybdenum disulfide with an ultraclean surface. Device mobilities and on/off ratios decrease linearly with the relative humidity varying from 0% to 35%, leading to a high sensitivity of more than 104 . The reversible water physisorption process leads to short response and decay times. In addition, the device array on a flexible substrate shows stable performance, suggesting great potential in future noncontact interface localization applications.

Thermally Activated Tunneling Transition in a Photoswitchable Single-Molecule Electrical Junction.

Exploring the charge transport process in molecular junctions is essential to the development of molecular electronics. Here, we investigate the temperature-dependent charge transport mechanism of carbon electrode-diarylethene single-molecule junctions, which possess photocontrollable molecular orbital energy levels due to reversible photoisomerization of individual diarylethenes between open and closed conformations. Both the experimental results and theoretical calculations consistently demonstrate that the vibronic coupling (thermally activated at the proper temperature) drives the transition of charge transport in the junctions from coherent tunneling to incoherent transport. Due to the subtle electron-phonon coupling effect, incoherent transport in the junctions proves to have different activation energies, depending on the photoswitchable molecular energy levels of two different conformations. These results improve fundamental understanding of charge transport mechanisms in molecular junctions and should lead to the rapid development of functional molecular devices toward practical applications.

Emergence of Tertiary Dirac Points in Graphene Moiré Superlattices.

The electronic structure of a crystalline solid is largely determined by its lattice structure. Recent advances in van der Waals solids, artificial crystals with controlled stacking of two-dimensional (2D) atomic films, have enabled the creation of materials with novel electronic structures. In particular, stacking graphene on hexagonal boron nitride (hBN) introduces a moiré superlattice that fundamentally modifies graphene's band structure and gives rise to secondary Dirac points (SDPs). Here we find that the formation of a moiré superlattice in graphene on hBN yields new, unexpected consequences: a set of tertiary Dirac points (TDPs) emerge, which give rise to additional sets of Landau levels when the sample is subjected to an external magnetic field. Our observations hint at the formation of a hidden Kekulé superstructure on top of the moiré superlattice under appropriate carrier doping and magnetic fields.

Stereoelectronic Effect-Induced Conductance Switching in Aromatic Chain Single-Molecule Junctions.

Biphenyl, as the elementary unit of organic functional materials, has been widely used in electronic and optoelectronic devices. However, over decades little has been fundamentally understood regarding how the intramolecular conformation of biphenyl dynamically affects its transport properties at the single-molecule level. Here, we establish the stereoelectronic effect of biphenyl on its electrical conductance based on the platform of graphene-molecule single-molecule junctions, where a specifically designed hexaphenyl aromatic chain molecule is covalently sandwiched between nanogapped graphene point contacts to create stable single-molecule junctions. Both theoretical and temperature-dependent experimental results consistently demonstrate that phenyl twisting in the aromatic chain molecule produces different microstates with different degrees of conjugation, thus leading to stochastic switching between high- and low-conductance states. These investigations offer new molecular design insights into building functional single-molecule electrical devices.

Covalently bonded single-molecule junctions with stable and reversible photoswitched conductivity.

Through molecular engineering, single diarylethenes were covalently sandwiched between graphene electrodes to form stable molecular conduction junctions. Our experimental and theoretical studies of these junctions consistently show and interpret reversible conductance photoswitching at room temperature and stochastic switching between different conductive states at low temperature at a single-molecule level. We demonstrate a fully reversible, two-mode, single-molecule electrical switch with unprecedented levels of accuracy (on/off ratio of ~100), stability (over a year), and reproducibility (46 devices with more than 100 cycles for photoswitching and ~10(5) to 10(6) cycles for stochastic switching).