Effects of gamma-ray irradiation on material and electrical properties of AlN gate dielectric on 4H-SiC.

This article investigates the radiation effects on as-deposited and annealed AlN films on 4H-SiC substrates under gamma-rays. The AlN films are prepared using plasma-enhanced-atomic-layer-deposition on an n-type 4H-SiC substrate. The AlN/4H-SiC MIS structure is subjected to gamma-ray irradiation with total doses of 0, 300, and 600 krad(Si). Physical, chemical, and electrical methods were employed to study the variations in surface morphology, charge transport, and interfacial trapping characteristics induced by irradiation. After 300 krad(Si) irradiation, the as-deposited and annealed samples exhibit their highest root mean square values of 0.917 nm and 1.190 nm, respectively, which is attributed to N vacancy defects induced by irradiation. Under irradiation, the flatband voltage (Vfb) of the as-deposited sample shifts from 2.24 to 0.78 V, while the annealed sample shifts from 1.18 to 2.16 V. X-ray photoelectron spectrum analysis reveals the decomposition of O-related defects in the as-deposited AlN and the formation of Al(NOx)ycompounds in the annealed sample. Furthermore, the space-charge-limits-conduction (SCLC) in the as-deposited sample is enhanced after radiation, while the barrier height of the annealed sample decreases from 1.12 to 0.84 eV, accompanied by the occurrence of the SCLC. The physical mechanism of the degradation of electrical performance in irradiated devices is the introduction of defects like N vacancies and O-related defects like Al(NOx)y. These findings provide valuable insights for SiC power devices in space applications.

Two-Dimensional Lateral Heterostructures Made by Selective Reaction on a Patterned Monolayer MoS2 Matrix.

Two-dimensional (2D) heterostructures have attracted widespread attention for their promising prospects in the fields of electronics and optoelectronics. However, in order to truly realize 2D-material-based integrated circuits, precisely controllable fabrication of 2D heterostructures is crucial and urgently needed. Here, we demonstrate an ex situ growth method of MoSe2/MoS2 lateral heterostructures by selective selenization of a laser-scanned, ultrathin oxidized region (MoOx) on a monolayer MoS2 matrix. In our method, monolayer MoS2 is scanned by a laser with a pre-designed pattern, where the laser-scanned MoS2 is totally oxidized into MoOx. The oxidized region is then selenized in a furnace, while the unoxidized MoS2 region remains unchanged, delivering a MoSe2/MoS2 heterostructure. Unlike in situ laser direct growth methods, our method separates the laser-scanned process from the selenization process, which avoids the long time of point-by-point selenization of MoS2 by laser, making the efficiency of the synthesis greatly improved. The formation process of the heterostructure is studied by Raman spectroscopy and Auger electron spectroscopy. This simple and controllable approach to lateral heterostructures with desired patterns paves the way for fast and mass integration of devices based on 2D heterostructures.

Enhanced Valley Splitting in Monolayer WSe2 by Phase Engineering.

Lifting the valley degeneracy in two-dimensional transition metal dichalcogenides could promote their applications in information processing. Various external regulations, including magnetic substrate, magnetic doping, electric field, and carrier doping, have been implemented to enhance the valley splitting under the magnetic field. Here, a phase engineering strategy, through modifying the intrinsic lattice structure, is proposed to enhance the valley splitting in monolayer WSe2. The valley splitting in hybrid H and T phase WSe2 is tunable by the concentration of the T phase. An obvious valley splitting of ∼4.1 meV is obtained with the T phase concentration of 31% under ±5 T magnetic fields, which corresponds to an effective Landé geff factor of -14, about 3.5-fold of that in pure H-WSe2. Comparing the temperature and magnetic field dependent polarized photoluminescence and also combining the theoretical simulations reveal the enhanced valley splitting is dominantly attributed to exchange interaction of H phase WSe2 with the local magnetic moments induced by the T phase. This finding provides a convenient solution for lifting the valley degeneracy of two-dimensional materials.

Heteromoiré Engineering on Magnetic Bloch Transport in Twisted Graphene Superlattices.

Localized electrons subject to applied magnetic fields can restart to propagate freely through the lattice in delocalized magnetic Bloch states (MBSs) when the lattice periodicity is commensurate with the magnetic length. Twisted graphene superlattices with moiré wavelength tunability enable experimental access to the unique delocalization in a controllable fashion. Here, we report the observation and characterization of high-temperature Brown-Zak (BZ) oscillations which come in two types, 1/B and B periodicity, originating from the generation of integer and fractional MBSs, in the twisted bilayer and trilayer graphene superlattices, respectively. Coexisting periodic-in-1/B oscillations assigned to different moiré wavelengths are dramatically observed in small-angle twisted bilayer graphene, which may arise from angle-disorder-induced in-plane heteromoiré superlattices. Moreover, the vertical stacking of heteromoiré supercells in double-twisted trilayer graphene results in a mega-sized superlattice. The exotic superlattice contributes to the periodic-in-B oscillation and dominates the magnetic Bloch transport.

An Anomalous Magneto-Optic Effect in Epitaxial Indium Selenide Layers.

Single-phonon modes offer potential applications in quantum phonon optics, but the phonon density of states of most materials consist of mixed contributions from coupled phonons. Here, using theoretical calculations and magneto-Raman measurements, we report two single-phonon vibration modes originating from the breathing and opposite out-of-plane vibrations of InSe layers. These single-phonon vibrations exhibit an anticorrelated scattering rotations of the polarization axis under an applied vertical magnetic field; such an anomalous magneto-optical behavior is due to the reverse bond polarizations of two quantum atomic vibrations, which induce different symmetry for the corresponding Raman selection rules. A 180° (+90° and -90°) integrated scattering rotation angle of two single-phonon modes was achieved when the magnetic field was swept from 0 to 6 T. This work demonstrates new ways to manipulate the magneto-optic effect through phonon polarity-based symmetry control and opens avenues for exploring single-phonon-vibration-based nanomechanical oscillators and magneto-phonon-coupled physics.

Room Temperature Commensurate Charge Density Wave on Epitaxially Grown Bilayer 2H-Tantalum Sulfide on Hexagonal Boron Nitride.

The breaking of multiple symmetries by periodic lattice distortion at a commensurate charge density wave (CDW) state is expected to give rise to intriguing interesting properties. However, accessing the commensurate CDW state on bulk TaS2 crystals typically requires cryogenic temperatures (77 K), which precludes practical applications. Here, we found that heteroepitaxial growth of a 2H-tantalum disulfide bilayer on a hexagonal-boron nitride (h-BN) substrate produces a robust commensurate CDW order at room temperature, characterized by a Moiré superlattice of 3 × 3 TaS2 on a 4 × 4 h-BN unit cell. The CDW order is confirmed by scanning transmission electron microscopy and Raman measurements. Theoretical calculations reveal that the stabilizing energy for the CDW phase of the monolayer and bilayer 2H-TaS2-on-h-BN substrates arises primarily from interfacial electrostatic interactions and, to a lesser extent, interfacial strain. Our work shows that engineering interfacial electrostatic interactions in an ultrathin van der Waals heterostructure constitutes an effective way to enhance CDW order in two-dimensional materials.

Molecular Beam Epitaxy of Highly Crystalline MoSe2 on Hexagonal Boron Nitride.

Molybdenum diselenide (MoSe2) is a promising two-dimensional material for next-generation electronics and optoelectronics. However, its application has been hindered by a lack of large-scale synthesis. Although chemical vapor deposition (CVD) using laboratory furnaces has been applied to grow two-dimensional (2D) MoSe2 cystals, no continuous film over macroscopically large area has been produced due to the lack of uniform control in these systems. Here, we investigate the molecular beam epitaxy (MBE) of 2D MoSe2 on hexagonal boron nitride (hBN) substrate, where highly crystalline MoSe2 film can be grown with electron mobility ∼15 cm2/(V s). Scanning transmission electron microscopy (STEM) shows that MoSe2 grains grown at an optimum temperature of 500 °C are highly oriented and coalesced to form continuous film with predominantly mirror twin boundaries. Our work suggests that van der Waals epitaxy of 2D materials is tolerant of lattice mismatch but is facilitated by substrates with similar symmetry.

Mo-Terminated Edge Reconstructions in Nanoporous Molybdenum Disulfide Film.

The catalytic and magnetic properties of molybdenum disulfide (MoS2) are significantly enhanced by the presence of edge sites. One way to obtain a high density of edge sites in a two-dimensional (2D) film is by introducing porosity. However, the large-scale bottom-up synthesis of a porous 2D MoS2 film remains challenging and the correlation of growth conditions to the atomic structures of the edges is not well understood. Here, using molecular beam epitaxy, we prepare wafer-scale nanoporous MoS2 films under conditions of high Mo flux and study their catalytic and magnetic properties. Atomic-resolution electron microscopy imaging of the pores reveals two new types of reconstructed Mo-terminated edges, namely, a distorted 1T (DT) edge and the Mo-Klein edge. Nanoporous MoS2 films are magnetic up to 400 K, which is attributed to the presence of Mo-terminated edges with unpaired electrons, as confirmed by density functional theory calculation. The small hydrogen adsorption free energy at these Mo-terminated edges leads to excellent activity for the hydrogen evolution reaction.

Valley Polarization of Trions and Magnetoresistance in Heterostructures of MoS2 and Yttrium Iron Garnet.

Manipulation of spin degree of freedom (DOF) of electrons is the fundamental aspect of spintronic and valleytronic devices. Two-dimensional transition metal dichalcogenides (2D TMDCs) exhibit an emerging valley pseudospin, in which spin-up (-down) electrons are distributed in a +K (-K) valley. This valley polarization gives a DOF for spintronic and valleytronic devices. Recently, magnetic exchange interactions between graphene and magnetic insulator yttrium iron garnet (YIG) have been exploited. However, the physics of 2D TMDCs with YIG have not been shown before. Here we demonstrate strong many-body effects in a heterostructure geometry comprising a MoS2 monolayer and YIG. High-order trions are directly identified by mapping absorption and photoluminescence at 12 K. The electron doping density is up to ∼1013 cm-2, resulting in a large splitting of ∼40 meV between trions and excitons. The trions exhibit a high circular polarization of ∼80% under optical pumping by circularly polarized light at ∼1.96 eV; it is confirmed experimentally that both phonon scattering and electron-hole exchange interaction contribute to the valley depolarization with temperature; importantly, a magnetoresistance (MR) behavior in the MoS2 monolayer was observed, and a giant MR ratio of ∼30% is achieved, which is 1 order of magnitude larger than the reported ratio in MoS2/CoFe2O4 heterostructures. Our experimental results confirm that the giant MR behaviors are attributed to the interfacial spin accumulation due to YIG substrates. Our work provides an insight into spin manipulation in a heterostructure of monolayer materials and magnetic substrates.

Molecular Beam Epitaxy of Highly Crystalline Monolayer Molybdenum Disulfide on Hexagonal Boron Nitride.

Atomically thin molybdenum disulfide (MoS2), a direct-band-gap semiconductor, is promising for applications in electronics and optoelectronics, but the scalable synthesis of highly crystalline film remains challenging. Here we report the successful epitaxial growth of a continuous, uniform, highly crystalline monolayer MoS2 film on hexagonal boron nitride (h-BN) by molecular beam epitaxy. Atomic force microscopy and electron microscopy studies reveal that MoS2 grown on h-BN primarily consists of two types of nucleation grains (0° aligned and 60° antialigned domains). By adopting a high growth temperature and ultralow precursor flux, the formation of 60° antialigned grains is largely suppressed. The resulting perfectly aligned grains merge seamlessly into a highly crystalline film. Large-scale monolayer MoS2 film can be grown on a 2 in. h-BN/sapphire wafer, for which surface morphology and Raman mapping confirm good spatial uniformity. Our study represents a significant step in the scalable synthesis of highly crystalline MoS2 films on atomically flat surfaces and paves the way to large-scale applications.

Chemical Vapor Deposition of Large-Size Monolayer MoSe2 Crystals on Molten Glass.

We report the fast growth of high-quality millimeter-size monolayer MoSe2 crystals on molten glass using an ambient pressure CVD system. We found that the isotropic surface of molten glass suppresses nucleation events and greatly improves the growth of large crystalline domains. Triangular monolayer MoSe2 crystals with sizes reaching ∼2.5 mm, and with a room-temperature carrier mobility up to ∼95 cm2/(V·s), can be synthesized in 5 min. The method can also be used to synthesize millimeter-size monolayer MoS2 crystals. Our results demonstrate that "liquid-state" glass is a highly promising substrate for the low-cost growth of high-quality large-size 2D transition metal dichalcogenides (TMDs).

Large Area Synthesis of 1D-MoSe2 Using Molecular Beam Epitaxy.

Large area synthesis of 1D-MoSe2 nanoribbons on both insulating and conducting substrates via molecular beam epitaxy is presented. Dimensional controlled growth of 2D, 1D-MoSe2 , and 1D-2D-MoSe2 hybrid heterostructure is achieved by tuning the growth temperature or Mo:Se precursor ratio.

Thermally Stable Mesoporous Perovskite Solar Cells Incorporating Low-Temperature Processed Graphene/Polymer Electron Transporting Layer.

In the short time since its discovery, perovskite solar cells (PSCs) have attained high power conversion efficiency but their lack of thermal stability remains a barrier to commercialization. Among the experimentally accessible parameter spaces for optimizing performance, identifying an electron transport layer (ETL) that forms a thermally stable interface with perovskite and which is solution-processable at low-temperature will certainly be advantageous. Herein, we developed a mesoporous graphene/polymer composite with these advantages when used as ETL in CH3NH3PbI3 PSCs, and a high efficiency of 13.8% under AM 1.5G solar illumination could be obtained. Due to the high heat transmission coefficient and low isoelectric point of mesoporous graphene-based ETL, the PSC device enjoys good chemical and thermal stability. Our work demonstrates that the mesoporous graphene-based scaffold is a promising ETL candidate for high performance and thermally stable PSCs.

Modulating Photoluminescence of Monolayer Molybdenum Disulfide by Metal-Insulator Phase Transition in Active Substrates.

The atomic thickness and flatness allow properties of 2D semiconductors to be modulated with influence from the substrate. Reversible modulation of these properties requires an "active," reconfigurable substrate, i.e., a substrate with switchable functionalities that interacts strongly with the 2D overlayer. In this work, the photoluminescence (PL) of monolayer molybdenum disulfide (MoS2 ) is modulated by interfacing it with a phase transition material, vanadium dioxide (VO2 ). The MoS2 PL intensity is enhanced by a factor of up to three when the underlying VO2 undergoes the thermally driven phase transition from the insulating to metallic phase. A nonvolatile, reversible way to rewrite the PL pattern is also demonstrated. The enhancement effect is attributed to constructive optical interference when the VO2 turns metallic. This modulation method requires no chemical or mechanical processes, potentially finding applications in new switches and sensors.

Achieving Ultrafast Hole Transfer at the Monolayer MoS2 and CH3NH3PbI3 Perovskite Interface by Defect Engineering.

The performance of a photovoltaic device is strongly dependent on the light harvesting properties of the absorber layer as well as the charge separation at the donor/acceptor interfaces. Atomically thin two-dimensional transition metal dichalcogenides (2-D TMDCs) exhibit strong light-matter interaction, large optical conductivity, and high electron mobility; thus they can be highly promising materials for next-generation ultrathin solar cells and optoelectronics. However, the short optical absorption path inherent in such atomically thin layers limits practical applications. A heterostructure geometry comprising 2-D TMDCs (e.g., MoS2) and a strongly absorbing material with long electron-hole diffusion lengths such as methylammonium lead halide perovskites (CH3NH3PbI3) may overcome this constraint to some extent, provided the charge transfer at the heterostructure interface is not hampered by their band offsets. Herein, we demonstrate that the intrinsic band offset at the CH3NH3PbI3/MoS2 interface can be overcome by creating sulfur vacancies in MoS2 using a mild plasma treatment; ultrafast hole transfer from CH3NH3PbI3 to MoS2 occurs within 320 fs with 83% efficiency following photoexcitation. Importantly, our work highlights the feasibility of applying defect-engineered 2-D TMDCs as charge-extraction layers in perovskite-based optoelectronic devices.

Ferroelectrically Gated Atomically Thin Transition-Metal Dichalcogenides as Nonvolatile Memory.

Ferroelectrically driven nonvolatile memory is demonstrated by interfacing 2D semiconductors and ferroelectric thin films, exhibiting superior memory performance comparable to existing thin-film ferroelectric field-effect transistors. An optical memory effect is also observed with large modulation of photoluminescence tuned by the ferroelectric gating, potentially finding applications in optoelectronics and valleytronics.

Self-Passivation of Defects: Effects of High-Energy Particle Irradiation on the Elastic Modulus of Multilayer Graphene.

The elastic modulus of multilayer graphene is found to be more robust to damage created by high-energy α-particle irradiation as compared to monolayer graphene. Theoretical analysis indicates that irradiation of multilayer graphene generates interlayer links that potentially increase the stiffness of the multilayer by passivating local defects.

Intensity tunable infrared broadband absorbers based on VO2 phase transition using planar layered thin films.

Plasmonic and metamaterial based nano/micro-structured materials enable spectrally selective resonant absorption, where the resonant bandwidth and absorption intensity can be engineered by controlling the size and geometry of nanostructures. Here, we demonstrate a simple, lithography-free approach for obtaining a resonant and dynamically tunable broadband absorber based on vanadium dioxide (VO2) phase transition. Using planar layered thin film structures, where top layer is chosen to be an ultrathin (20 nm) VO2 film, we demonstrate broadband IR light absorption tuning (from ~90% to ~30% in measured absorption) over the entire mid-wavelength infrared spectrum. Our numerical and experimental results indicate that the bandwidth of the absorption bands can be controlled by changing the dielectric spacer layer thickness. Broadband tunable absorbers can find applications in absorption filters, thermal emitters, thermophotovoltaics and sensing.

MoS2 Heterojunctions by Thickness Modulation.

In this work, we report lateral heterojunction formation in as-exfoliated MoS2 flakes by thickness modulation. Kelvin probe force microscopy is used to map the surface potential at the monolayer-multilayer heterojunction, and consequently the conduction band offset is extracted. Scanning photocurrent microscopy is performed to investigate the spatial photocurrent response along the length of the device including the source and the drain contacts as well as the monolayer-multilayer junction. The peak photocurrent is measured at the monolayer-multilayer interface, which is attributed to the formation of a type-I heterojunction. The work presents experimental and theoretical understanding of the band alignment and photoresponse of thickness modulated MoS2 junctions with important implications for exploring novel optoelectronic devices.

Simultaneous Enhancement of Electrical Conductivity and Thermopower of Bi2Te3 by Multifunctionality of Native Defects.

Simultaneous increases in electrical conductivity (up to 200%) and thermopower (up to 70%) are demonstrated by introducing native defects in Bi2 Te3 films, leading to a high power factor of 3.4 × 10(-3) W m(-1) K(-2). The maximum enhancement of the power factor occurs when the native defects act beneficially both as electron donors and energy filters to mobile electrons. They also act as effective phonon scatterers.