Gyeong Hee Ryu

Fast Synthesis of High-Performance Graphene Films by Hydrogen-Free Rapid Thermal Chemical Vapor Deposition

The practical use of graphene in consumer electronics has not been demonstrated since the size, uniformity, and reliability problems are yet to be solved to satisfy industrial standards. Here we report mass-produced graphene films synthesized by hydrogen-free rapid thermal chemical vapor deposition (RT-CVD), roll-to-roll etching, and transfer methods, which enabled faster and larger production of homogeneous graphene films over 400 × 300 mm(2) area with a sheet resistance of 249 ± 17 Ω/sq without additional doping. The properties of RT-CVD graphene have been carefully characterized by high-resolution transmission electron microscopy, Raman spectroscopy, chemical grain boundary analysis, and various electrical device measurements, showing excellent uniformity and stability. In particular, we found no significant correlation between graphene domain sizes and electrical conductivity, unlike previous theoretical expectations for nanoscale graphene domains. Finally, the actual application of the RT-CVD films to capacitive multitouch devices installed in the most sophisticated mobile phone was demonstrated.

Synthesis of wafer-scale uniform molybdenum disulfide films with control over the layer number using a gas phase sulfur precursor

We describe a method for synthesizing large-area and uniform molybdenum disulfide films, with control over the layer number, on insulating substrates using a gas phase sulfuric precursor (H2S) and a molybdenum metal source. The metal layer thickness was varied to effectively control the number of layers (2 to 12) present in the synthesized film. The films were grown on wafer-scale Si/SiO2 or quartz substrates and displayed excellent uniformity and a high crystallinity over the entire area. Thin film transistors were prepared using these materials, and the performances of the devices were tested. The devices displayed an on/off current ratio of 10(5), a mobility of 0.12 cm(2) V(-1) s(-1) (mean mobility value of 0.07 cm(2) V(-1) s(-1)), and reliable operation.

Direct exfoliation and dispersion of two-dimensional materials in pure water via temperature control

The high-volume synthesis of two-dimensional (2D) materials in the form of platelets is desirable for various applications. While water is considered an ideal dispersion medium, due to its abundance and low cost, the hydrophobicity of platelet surfaces has prohibited its widespread use. Here we exfoliate 2D materials directly in pure water without using any chemicals or surfactants. In order to exfoliate and disperse the materials in water, we elevate the temperature of the sonication bath, and introduce energy via the dissipation of sonic waves. Storage stability greater than one month is achieved through the maintenance of high temperatures, and through atomic and molecular level simulations, we further discover that good solubility in water is maintained due to the presence of platelet surface charges as a result of edge functionalization or intrinsic polarity. Finally, we demonstrate inkjet printing on hard and flexible substrates as a potential application of water-dispersed 2D materials.

Controllable synthesis of molybdenum tungsten disulfide alloy for vertically composition-controlled multilayer

The effective synthesis of two-dimensional transition metal dichalcogenides alloy is essential for successful application in electronic and optical devices based on a tunable band gap. Here we show a synthesis process for Mo1−xWxS2 alloy using sulfurization of super-cycle atomic layer deposition Mo1−xWxOy. Various spectroscopic and microscopic results indicate that the synthesized Mo1−xWxS2 alloys have complete mixing of Mo and W atoms and tunable band gap by systematically controlled composition and layer number. Based on this, we synthesize a vertically composition-controlled (VCC) Mo1−xWxS2 multilayer using five continuous super-cycles with different cycle ratios for each super-cycle. Angle-resolved X-ray photoemission spectroscopy, Raman and ultraviolet–visible spectrophotometer results reveal that a VCC Mo1−xWxS2 multilayer has different vertical composition and broadband light absorption with strong interlayer coupling within a VCC Mo1−xWxS2 multilayer. Further, we demonstrate that a VCC Mo1−xWxS2 multilayer photodetector generates three to four times greater photocurrent than MoS2- and WS2-based devices, owing to the broadband light absorption.

Low‐Temperature Synthesis of Large‐Scale Molybdenum Disulfide Thin Films Directly on a Plastic Substrate Using Plasma‐Enhanced Chemical Vapor Deposition

By plasma-enhanced chemical vapor deposition, a molybdenum disulfide (MoS2 ) thin film is synthesized directly on a wafer-scale plastic substrate at below 300 °C. The carrier mobility of the films is 3.74 cm(2) V(-1) s(-1) . Also, humidity is successfully detected with MoS2 -based sensors fabricated on the flexible substrate, which reveals its potential for flexible sensing devices.

Interface-Controlled Synthesis of Heterodimeric Silver–Carbon Nanoparticles Derived from Polysaccharides

Hybrid nanoparticles composed of multiple components can offer unique opportunities for understanding the nanoscale mechanism and advanced material applications. Here, we report the synthesis of heterodimeric silver-carbon dot nanoparticles (Ag-CD NPs) where the Ag NP is grown on the surface of CDs derived from polysaccharides, such as chitosan and alginate, through the photoelectron transfer reaction between CD and Ag(+) ions. The nanoscale interface between the Ag NPs and the CDs is highly tunable depending on the precursor of the CDs and the amount of additives, resulting in fine modification of photoluminescence of the CDs as well as the related surface plasmon resonance of the Ag NPs. This result demonstrates the critical role of the interface between the hybrid nanoparticles in governing the electrical and optical properties of respective nanoparticles.

Raman Signatures of Polytypism in Molybdenum Disulfide

Since the stacking order sensitively affects various physical properties of layered materials, accurate determination of the stacking order is important for studying the basic properties of these materials as well as for device applications. Because 2H-molybdenum disulfide (MoS2) is most common in nature, most studies so far have focused on 2H-MoS2. However, we found that the 2H, 3R, and mixed stacking sequences exist in few-layer MoS2 exfoliated from natural molybdenite crystals. The crystal structures are confirmed by HR-TEM measurements. The Raman signatures of different polytypes are investigated by using three different excitation energies that are nonresonant and resonant with A and C excitons, respectively. The low-frequency breathing and shear modes show distinct differences for each polytype, whereas the high-frequency intralayer modes show little difference. For resonant excitations at 1.96 and 2.81 eV, distinct features are observed that enable determination of the stacking order.

Monolithic graphene oxide sheets with controllable composition

Graphene oxide potentially has multiple applications and is typically prepared by solution-based chemical means. To date, the synthesis of a monolithic form of graphene oxide that is crucial to the precision assembly of graphene-based devices has not been achieved. Here we report the physical approach to produce monolithic graphene oxide sheets on copper foil using solid carbon, with tunable oxygen-to-carbon composition. Experimental and theoretical studies show that the copper foil provides an effective pathway for carbon diffusion, trapping the oxygen species dissolved in copper and enabling the formation of monolithic graphene oxide sheets. Unlike chemically derived graphene oxide, the as-synthesized graphene oxide sheets are electrically active, and the oxygen-to-carbon composition can be tuned during the synthesis process. As a result, the resulting graphene oxide sheets exhibit tunable bandgap energy and electronic properties. Our solution-free, physical approach may provide a path to a new class of monolithic, two-dimensional chemically modified carbon sheets.

Self-Limiting Layer Synthesis of Transition Metal Dichalcogenides.

This work reports the self-limiting synthesis of an atomically thin, two dimensional transition metal dichalcogenides (2D TMDCs) in the form of MoS2. The layer controllability and large area uniformity essential for electronic and optical device applications is achieved through atomic layer deposition in what is named self-limiting layer synthesis (SLS); a process in which the number of layers is determined by temperature rather than process cycles due to the chemically inactive nature of 2D MoS2. Through spectroscopic and microscopic investigation it is demonstrated that SLS is capable of producing MoS2 with a wafer-scale (~10 cm) layer-number uniformity of more than 90%, which when used as the active layer in a top-gated field-effect transistor, produces an on/off ratio as high as 108. This process is also shown to be applicable to WSe2, with a PN diode fabricated from a MoS2/WSe2 heterostructure exhibiting gate-tunable rectifying characteristics.

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.