Kenji Kawahara

Large-scale synthesis of NbS2 nanosheets with controlled orientation on graphene by ambient pressure CVD

We report ambient pressure chemical vapor deposition (CVD) growth of single-crystalline NbS2 nanosheets with controlled orientation. On Si and SiO2 substrates, NbS2 nanosheets grow almost perpendicular to the substrate surface. However, when we apply transferred CVD graphene on SiO2 as a substrate, NbS2 sheets grow laterally lying on the graphene. The NbS2 sheets show the triangular and hexagonal shapes with a thickness of about 20-200 nm and several micrometres in the lateral dimension. Analyses based on X-ray diffraction and Raman spectroscopy indicate that the NbS2 nanosheets are single crystalline 3R-type with a rhombohedral structure of R3m space group. Our findings on the formation of highly aligned NbS2 nanosheets on graphene give new insight into the formation mechanism of NbS2 and would contribute to the templated growth of various layered materials.

Epitaxial growth and electronic properties of large hexagonal graphene domains on Cu(111) thin film

Large hexagonal single-crystalline domains of single-layer graphene are epitaxially grown by ambient-pressure chemical vapor deposition over a thin Cu(111) film deposited on c-plane sapphire. The hexagonal graphene domains with a maximum size of 100 µm are oriented in the same direction due to the epitaxial growth. Reflecting high crystallinity, a clear band structure with the Dirac cone is observed by angle-resolved photoelectron spectroscopy (ARPES), and a high carrier mobility exceeding 4,000 cm2 V-1 s-1 is obtained on SiO2/Si at room temperature. Our epitaxial approach combined with large domain growth is expected to contribute to future electronic applications.

Structure and transport properties of the interface between CVD-grown graphene domains.

During the chemical vapor deposition (CVD) growth of graphene, graphene domains grown on a Cu surface merge together and form a uniform graphene sheet. For high-performance electronics and other applications, it is important to understand the interfacial structure of the merged domains, as well as their influence on the physical properties of graphene. We synthesized large hexagonal graphene domains with controlled orientations on a heteroepitaxial Cu film and studied the structure and properties of the interfaces between the domains mainly merged with the same angle. Although the merged domains have various interfaces with/without wrinkles and/or increased defect-related Raman D-band intensity, the intra-domain transport showed higher carrier mobility reaching 20,000 cm(2) V(-1) s(-1) on SiO2 at 280 K (the mean value was 7200 cm(2) V(-1) s(-1)) than that measured for inter-domain areas, 6400 cm(2) V(-1) s(-1) (mean value 2000 cm(2) V(-1) s(-1)). The temperature dependence of the mobility suggests that impurity scattering dominates at the interface even for the merged domains with the same orientation. This study highlights the importance of domain interfaces, especially on the carrier transport properties, in CVD-grown graphene.

Dynamically generated pure spin current in single-layer graphene

The conductance mismatch problem limits the spin-injection efficiency significantly, and spin-injection into graphene has been usually requiring high-quality tunnel barriers to circumvent the conductance mismatch. We introduce a novel approach, which enables generation of a pure spin current into single-layer graphene (SLG) free from electrical conductance mismatch by using dynamical spin injection. Experimental demonstration of spin-pumping-induced spin current generation and spin transport in SLG at room temperature was successfully achieved and the spin coherence was estimated to be 1.36 {\mu}m by using a conventional theoretical model based on Landau-Lifshitz-Gilbert equation. The spin coherence is proportional to the quality of SLG, which indicates that spin relaxation in SLG is governed by the Elliot-Yafet mechanism as was reported.

Gate-Tunable Spin-Charge Conversion and the Role of Spin-Orbit Interaction in Graphene

The small spin-orbit interaction of carbon atoms in graphene promises a long spin diffusion length and the potential to create a spin field-effect transistor. However, for this reason, graphene was largely overlooked as a possible spin-charge conversion material. We report electric gate tuning of the spin-charge conversion voltage signal in single-layer graphene. Using spin pumping from an yttrium iron garnet ferrimagnetic insulator and ionic liquid top gate, we determined that the inverse spin Hall effect is the dominant spin-charge conversion mechanism in single-layer graphene. From the gate dependence of the electromotive force we showed the dominance of the intrinsic over Rashba spin-orbit interaction, a long-standing question in graphene research.

Temperature dependent thermal conductivity of a suspended submicron graphene ribbon

Thermophysical characterization of graphene is very important for both fundamental and technological research. While most of the existing thermal conductivity measurements are for graphene sheets with sizes larger than 1 μm, the thermal conductivities for suspended submicron graphene ribbons are still very few, although the thermal conductivity of graphene ribbons at the submicron scale is predicted to be much smaller than large graphene and strongly size dependent for both length and width due to the 2D nature of phonon transport. Here, we report the temperature dependent thermal conductivity of a 169-nm wide and 846-nm long graphene ribbon measured by the electrical self-heating method. The measured thermal conductivities range from (12.7 ± 2.95) W/m/K at 80 K to (932 ± 333) W/m/K at 380 K, being (349 ± 63) W/m/K at 300 K, following a ∼ T2.79 law for the full temperature range of 80 K to 380 K and a ∼ T1.23 law at low temperatures. The comparison of the measured thermal conductance with the ballistic tr...

Observation of spin-charge conversion in chemical-vapor-deposition-grown single-layer graphene

Conversion of pure spin current to charge current in single-layer graphene (SLG) is investigated by using spin pumping. Large-area SLG grown by chemical vapor deposition is used for the conversion. Efficient spin accumulation in SLG by spin pumping enables observing an electromotive force produced by the inverse spin Hall effect (ISHE) of SLG. The spin Hall angle of SLG is estimated to be 6.1*10-7. The observed ISHE in SLG is ascribed to its non-negligible spin-orbit interaction in SLG.

Highly Conductive and Transparent Large‐Area Bilayer Graphene Realized by MoCl5 Intercalation

Bilayer graphene (BLG) comprises a 2D nanospace sandwiched by two parallel graphene sheets that can be used to intercalate molecules or ions for attaining novel functionalities. However, intercalation is mostly demonstrated with small, exfoliated graphene flakes. This study demonstrates intercalation of molybdenum chloride (MoCl5 ) into a large-area, uniform BLG sheet, which is grown by chemical vapor deposition (CVD). This study reveals that the degree of MoCl5 intercalation strongly depends on the stacking order of the graphene; twist-stacked graphene shows a much higher degree of intercalation than AB-stacked. Density functional theory calculations suggest that weak interlayer coupling in the twist-stacked graphene contributes to the effective intercalation. By selectively synthesizing twist-rich BLG films through control of the CVD conditions, low sheet resistance (83 Ω ▫-1 ) is realized after MoCl5 intercalation, while maintaining high optical transmittance (≈95%). The low sheet resistance state is relatively stable in air for more than three months. Furthermore, the intercalated BLG film is applied to organic solar cells, realizing a high power conversion efficiency.

High-speed and on-chip graphene blackbody emitters for optical communications by remote heat transfer

High-speed light emitters integrated on silicon chips can enable novel architectures for silicon-based optoelectronics, such as on-chip optical interconnects, and silicon photonics. However, conventional light sources based on compound semiconductors face major challenges for their integration with a silicon-based platform because of their difficulty of direct growth on a silicon substrate. Here we report ultra-high-speed (100-ps response time), highly integrated graphene-based on-silicon-chip blackbody emitters in the near-infrared region including telecommunication wavelength. Their emission responses are strongly affected by the graphene contact with the substrate depending on the number of graphene layers. The ultra-high-speed emission can be understood by remote quantum thermal transport via surface polar phonons of the substrates. We demonstrated real-time optical communications, integrated two-dimensional array emitters, capped emitters operable in air, and the direct coupling of optical fibers to the emitters. These emitters can open new routes to on-Si-chip, small footprint, and high-speed emitters for highly integrated optoelectronics and silicon photonics.Integrating graphene with existing silicon technologies may pave the way to compact light sources for optoelectronics and photonics. Here, the authors fabricate graphene-based arrays of blackbody emitters integrated on a silicon chip, operating in the near-infrared region at high speed.

Moisture barrier properties of single-layer graphene deposited on Cu films for Cu metallization

The moisture barrier properties of large-grain single-layer graphene (SLG) deposited on a Cu(111)/sapphire substrate are demonstrated by comparing with the bare Cu(111) surface under an accelerated degradation test (ADT) at 85 °C and 85% relative humidity (RH) for various durations. The change in surface color and the formation of Cu oxide are investigated by optical microscopy (OM) and X-ray photoelectron spectroscopy (XPS), respectively. First-principle simulation is performed to understand the mechanisms underlying the barrier properties of SLG against O diffusion. The correlation between Cu oxide thickness and SLG quality are also analyzed by spectroscopic ellipsometry (SE) measured on a non-uniform SLG film. SLG with large grains shows high performance in preventing the Cu oxidation due to moisture during ADT.