A-Rang Jang

Growth of High-Crystalline, Single-Layer Hexagonal Boron Nitride on Recyclable Platinum Foil

Hexagonal boron nitride (h-BN) is gaining significant attention as a two-dimensional dielectric material, along with graphene and other such materials. Herein, we demonstrate the growth of highly crystalline, single-layer h-BN on Pt foil through a low-pressure chemical vapor deposition method that allowed h-BN to be grown over a wide area (8 × 25 mm(2)). An electrochemical bubbling-based method was used to transfer the grown h-BN layer from the Pt foil onto an arbitrary substrate. This allowed the Pt foil, which was not consumed during the process, to be recycled repeatedly. The UV-visible absorption spectrum of the single-layer h-BN suggested an optical band gap of 6.06 eV, while a high-resolution transmission electron microscopy image of the same showed the presence of distinct hexagonal arrays of B and N atoms, which were indicative of the highly crystalline nature and single-atom thickness of the h-BN layer. This method of growing single-layer h-BN over large areas was also compatible with use of a sapphire substrate.

Probing Evolution of Twist-Angle-Dependent Interlayer Excitons in MoSe2/WSe2 van der Waals Heterostructures

Interlayer excitons were observed at the heterojunctions in van der Waals heterostructures (vdW HSs). However, it is not known how the excitonic phenomena are affected by the stacking order. Here, we report twist-angle-dependent interlayer excitons in MoSe2/WSe2 vdW HSs based on photoluminescence (PL) and vdW-corrected density functional theory calculations. The PL intensity of the interlayer excitons depends primarily on the twist angle: It is enhanced at coherently stacked angles of 0° and 60° (owing to strong interlayer coupling) but disappears at incoherent intermediate angles. The calculations confirm twist-angle-dependent interlayer coupling: The states at the edges of the valence band exhibit a long tail that stretches over the other layer for coherently stacked angles; however, the states are largely confined in the respective layers for intermediate angles. This interlayer hybridization of the band edge states also correlates with the interlayer separation between MoSe2 and WSe2 layers. Furthermore, the interlayer coupling becomes insignificant, irrespective of twist angles, by the incorporation of a hexagonal boron nitride monolayer between MoSe2 and WSe2.

Support-Free Transfer of Ultrasmooth Graphene Films Facilitated by Self-Assembled Monolayers for Electronic Devices and Patterns

We explored a support-free method for transferring large area graphene films grown by chemical vapor deposition to various fluoric self-assembled monolayer (F-SAM) modified substrates including SiO2/Si wafers, polyethylene terephthalate films, and glass. This method yields clean, ultrasmooth, and high-quality graphene films for promising applications such as transparent, conductive, and flexible films due to the absence of residues and limited structural defects such as cracks. The F-SAM introduced in the transfer process can also lead to graphene transistors with enhanced field-effect mobility (up to 10,663 cm(2)/Vs) and resistance modulation (up to 12×) on a standard silicon dioxide dielectric. Clean graphene patterns can be realized by transfer of graphene onto only the F-SAM modified surfaces.

Stress-induced domain dynamics and phase transitions in epitaxially grown VO₂ nanowires.

We demonstrate that surface stresses in epitaxially grown VO₂ nanowires (NWs) have a strong effect on the appearance and stability of intermediate insulating M₂ phases, as well as the spatial distribution of insulating and metallic domains during structural phase transitions. During the transition from an insulating M1 phase to a metallic R phase, the coexistence of insulating M₁ and M₂ phases with the absence of a metallic R phase was observed at atmospheric pressure. In addition, we show that, for a VO₂ NW without the presence of an epitaxial interface, surface stresses dominantly lead to spatially inhomogeneous phase transitions between insulating and metallic phases. In contrast, for a VO₂ NW with the presence of an epitaxial interface, the strong epitaxial interface interaction leads to additional stresses resulting in uniformly alternating insulating and metallic domains along the NW length.

Catalytic Conversion of Hexagonal Boron Nitride to Graphene for In-Plane Heterostructures

Heterostructures of hexagonal boron nitride (h-BN) and graphene have attracted a great deal of attention for potential applications in 2D materials. Although several methods have been developed to produce this material through the partial substitution reaction of graphene, the reverse reaction has not been reported. Though the endothermic nature of this reaction might account for the difficulty and previous absence of such a process, we report herein a new chemical route in which the Pt substrate plays a catalytic role. We propose that this reaction proceeds through h-BN hydrogenation; subsequent graphene growth quickly replaces the initially etched region. Importantly, this conversion reaction enables the controlled formation of patterned in-plane graphene/h-BN heterostructures, without needing the commonly employed protecting mask, simply by using a patterned Pt substrate.

Strain-mediated interlayer coupling effects on the excitonic behaviors in an epitaxially-grown MoS2/WS2 van der Waals heterobilayer

van der Waals heterostructures composed of two different monolayer crystals have recently attracted attention as a powerful and versatile platform for studying fundamental physics, as well as having great potential in future functional devices because of the diversity in the band alignments and the unique interlayer coupling that occurs at the heterojunction interface. However, despite these attractive features, a fundamental understanding of the underlying physics accounting for the effect of interlayer coupling on the interactions between electrons, photons, and phonons in the stacked heterobilayer is still lacking. Here, we demonstrate a detailed analysis of the strain-dependent excitonic behavior of an epitaxially grown MoS2/WS2 vertical heterostructure under uniaxial tensile and compressive strain that enables the interlayer interactions to be modulated along with the electronic band structure. We find that the strain-modulated interlayer coupling directly affects the characteristic combined vibrational and excitonic properties of each monolayer in the heterobilayer. It is further revealed that the relative photoluminescence intensity ratio of WS2 to MoS2 in our heterobilayer increases monotonically with tensile strain and decreases with compressive strain. We attribute the strain-dependent emission behavior of the heterobilayer to the modulation of the band structure for each monolayer, which is dictated by the alterations in the band gap transitions. These findings present an important pathway toward designing heterostructures and flexible devices.

Thermodynamically Stable Synthesis of Large‐Scale and Highly Crystalline Transition Metal Dichalcogenide Monolayers and their Unipolar n–n Heterojunction Devices

Transition metal dichalcogenide (TMDC) monolayers are considered to be potential materials for atomically thin electronics due to their unique electronic and optical properties. However, large-area and uniform growth of TMDC monolayers with large grain sizes is still a considerable challenge. This report presents a simple but effective approach for large-scale and highly crystalline molybdenum disulfide monolayers using a solution-processed precursor deposition. The low supersaturation level, triggered by the evaporation of an extremely thin precursor layer, reduces the nucleation density dramatically under a thermodynamically stable environment, yielding uniform and clean monolayer films and large crystal sizes up to 500 µm. As a result, the photoluminescence exhibits only a small full-width-half-maximum of 48 meV, comparable to that of exfoliated and suspended monolayer crystals. It is confirmed that this growth procedure can be extended to the synthesis of other TMDC monolayers, and robust MoS2 /WS2 heterojunction devices are easily prepared using this synthetic procedure due to the large-sized crystals. The heterojunction device shows a fast response time (≈45 ms) and a significantly high photoresponsivity (≈40 AW-1 ) because of the built-in potential and the majority-carrier transport at the n-n junction. These findings indicate an efficient pathway for the fabrication of high-performance 2D optoelectronic devices.

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.

Hydrogenation of monolayer molybdenum diselenide via hydrogen plasma treatment

Functionalization of transition metal dichalcogenides has been studied with the aim of tuning their electrical and optical properties, but structural information during functionalization and its reversibility have not been elucidated. We report a simple and effective method for hydrogenation of monolayer MoSe2 using hydrogen plasma treatment. The covalent bonding of hydrogen to MoSe2 was confirmed by X-ray photoelectron spectroscopy, and the degree of hydrogenation was modulated from 32% to 80% by increasing the plasma treatment time from 5 to 40 s. Transmission electron microscopy confirmed a 1.5% reduction in the lattice constant of hydrogenated MoSe2 without structural damages or defects; crystal structures of hydrogenated MoSe2 and as-prepared MoSe2 were identical. Photoluminescence (PL) investigation of hydrogenated MoSe2 showed charge transfer from hydrogen to MoSe2. Furthermore, reversible desorption of hydrogen from hydrogenated MoSe2 was achieved by heat treatment. The optical and electrical properties of as-prepared and hydrogenated MoSe2 samples were compared. The PL peak of hydrogenated MoSe2 returned to the as-prepared one after heat treatment at 500 °C. Furthermore, the electron mobility of MoSe2 decreased from 29 to 9 cm2 V−1 s−1 after hydrogenation and was restored to 27 cm2 V−1 s−1 upon heat treatment at 500 °C. This reversible hydrogen adsorption and desorption lends control over the optical and electrical properties of monolayer MoSe2 and contributes to the hydrogen functionalization of monolayer transition metal dichalcogenides and other two-dimensional materials.

Balancing Charge Carrier Transport in a Quantum Dot P–N Junction toward Hysteresis-Free High-Performance Solar Cells

In a quantum dot solar cell (QDSC) that has an inverted structure, the QD layers form two different junctions between the electron transport layer (ETL) and the other semiconducting QD layer. Recent work on an inverted-structure QDSC has revealed that the junction between the QD layers is the dominant junction, rather than the junction between the ETL and the QD layers, which is in contrast to the conventional wisdom. However, to date, there have been a lack of systematic studies on the role and importance of the QD heterojunction structure on the behavior of the solar cell and the resulting device performance. In this study, we have systematically controlled the structure of the QD junction to balance charge transport, which demonstrates that the position of the junction has a significant effect on the hysteresis effect, fill factor, and solar cell performance and is attributed to balanced charge transport.