The controlled synthesis of highly crystalline MoS2 atomic layers remains a challenge for the practical applications of this emerging material. Here, we developed an approach for synthesizing MoS2 ...flakes in rhomboid shape with controlled number of layers by the layer-by-layer sulfurization of MoO2 microcrystals. The obtained MoS2 flakes showed high crystallinity with crystal domain size of ∼10 μm, significantly larger than the grain size of MoS2 grown by other methods. As a result of the high crystallinity, the performance of back-gated field effect transistors (FETs) made on these MoS2 flakes was comparable to that of FETs based on mechanically exfoliated flakes. This simple approach opens up a new avenue for controlled synthesis of MoS2 atomic layers and will make this highly crystalline material easily accessible for fundamental aspects and various applications.
Graphene nanoribbons (GNRs) are materials with properties distinct from those of other carbon allotropes. The all-semiconducting nature of sub-10-nm GNRs could bypass the problem of the extreme ...chirality dependence of the metal or semiconductor nature of carbon nanotubes (CNTs) in future electronics. Currently, making GNRs using lithographic, chemical or sonochemical methods is challenging. It is difficult to obtain GNRs with smooth edges and controllable widths at high yields. Here we show an approach to making GNRs by unzipping multiwalled carbon nanotubes by plasma etching of nanotubes partly embedded in a polymer film. The GNRs have smooth edges and a narrow width distribution (10-20 nm). Raman spectroscopy and electrical transport measurements reveal the high quality of the GNRs. Unzipping CNTs with well-defined structures in an array will allow the production of GNRs with controlled widths, edge structures, placement and alignment in a scalable fashion for device integration.
Graphene nanoribbons have attracted attention because of their novel electronic and spin transport properties, and also because nanoribbons less than 10 nm wide have a bandgap that can be used to ...make field-effect transistors. However, producing nanoribbons of very high quality, or in high volumes, remains a challenge. Here, we show that pristine few-layer nanoribbons can be produced by unzipping mildly gas-phase oxidized multiwalled carbon nanotubes using mechanical sonication in an organic solvent. The nanoribbons are of very high quality, with smooth edges (as seen by high-resolution transmission electron microscopy), low ratios of disorder to graphitic Raman bands, and the highest electrical conductance and mobility reported so far (up to 5e(2)/h and 1,500 cm(2) V(-1) s(-1) for ribbons 10-20 nm in width). Furthermore, at low temperatures, the nanoribbons show phase-coherent transport and Fabry-Perot interference, suggesting minimal defects and edge roughness. The yield of nanoribbons is approximately 2% of the starting raw nanotube soot material, significantly higher than previous methods capable of producing high-quality narrow nanoribbons. The relatively high-yield synthesis of pristine graphene nanoribbons will make these materials easily accessible for a wide range of fundamental and practical applications.
We devised a controlled hydrogen plasma reaction at 300 °C to etch graphene and graphene nanoribbons (GNRs) selectively at the edges over the basal plane. Atomic force microscope imaging showed that ...the etching rates for single-layer and few-layer (≥2 layers) graphene are 0.27 ± 0.05 nm/min and 0.10 ± 0.03 nm/min, respectively. Meanwhile, Raman spectroscopic mapping revealed no D band in the planes of single-layer or few-layer graphene after the plasma reaction, suggesting selective etching at the graphene edges without introducing defects in the basal plane. We found that hydrogen plasma at lower temperature (room temperature) or a higher temperature (500 °C) could hydrogenate the basal plane or introduce defects in the basal plane. Using the hydrogen plasma reaction at the intermediate temperature (300 °C), we obtained narrow, presumably hydrogen terminated GNRs (sub-5 nm) by etching of wide GNRs derived from unzipping of multiwalled carbon nanotubes. Such GNRs exhibited semiconducting characteristics with high on/off ratios (∼1000) in GNR field effect transistor devices at room temperature.
Two-dimensional atomic crystals, such as two-dimensional oxides, have attracted much attention in energy storage because nearly all of the atoms can be exposed to the electrolyte and involved in ...redox reactions. However, current strategies are largely limited to intrinsically layered compounds. Here we report a general strategy that uses the surfaces of water-soluble salt crystals as growth templates and is applicable to not only layered compounds but also various transition metal oxides, such as hexagonal-MoO3, MoO2, MnO and hexagonal-WO3. The planar growth is hypothesized to occur via a match between the crystal lattices of the salt and the growing oxide. Restacked two-dimensional hexagonal-MoO3 exhibits high pseudocapacitive performances (for example, 300 F cm(-3) in an Al2(SO4)3 electrolyte). The synthesis of various two-dimensional transition metal oxides and the demonstration of high capacitance are expected to enable fundamental studies of dimensionality effects on their properties and facilitate their use in energy storage and other applications.
Developing controlled approaches for synthesizing high‐quality two‐dimensional (2D) semiconductors is essential for their practical applications in novel electronics. The application of chemical ...vapor transport (CVT), an old single‐crystal growth technique, has been extended from growing 3D crystals to synthesizing 2D atomic layers by tuning the growth kinetics. Both single crystalline individual flakes and continuous films of 1 L MoS2 were successfully obtained with CVT approach at low growth temperatures of 300–600 °C. The obtained 1 L MoS2 exhibits high crystallinity and comparable mobility to mechanically exfoliated samples, as confirmed by both atomic resolution microscopic imaging and electrical transport measurements. Besides MoS2, this method was also used in the growth of 2D WS2, MoSe2, MoxW1−xS2 alloys, and ReS2, thus opening up a new way for the controlled synthesis of various 2D semiconductors.
Layer by layer: The controllable synthesis of highly crystalline two‐dimensional (2D) semiconducting atomic layers has been achieved by using an old crystal growth technique, chemical vapor transport. This approach opens a new avenue for the chemical synthesis of high‐quality 2D semiconductors.
Two‐dimensional (2D) PtSe2 shows the most prominent layer‐dependent electrical properties among various 2D materials and high catalytic activity for hydrogen evolution reaction (HER), and therefore, ...it is an ideal material for exploring the structure–activity correlations in 2D systems. Here, starting with the synthesis of single‐crystalline 2D PtSe2 with a controlled number of layers and probing the HER catalytic activity of individual flakes in micro electrochemical cells, we investigated the layer‐dependent HER catalytic activity of 2D PtSe2 from both theoretical and experimental perspectives. We clearly demonstrated how the number of layers affects the number of active sites, the electronic structures, and electrical properties of 2D PtSe2 flakes and thus alters their catalytic performance for HER. Our results also highlight the importance of efficient electron transfer in achieving optimum activity for ultrathin electrocatalysts. Our studies greatly enrich our understanding of the structure–activity correlations for 2D catalysts and provide new insight for the design and synthesis of ultrathin catalysts with high activity.
Through thick and thin: Since the thickness of two‐dimensional (2D) PtSe2 flakes can be controlled by adjusting synthesis conditions, their layer‐dependent catalytic activity for the hydrogen evolution reaction could be investigated from both theoretical and experimental perspectives. Structure–activity correlations were drawn, providing new insights for the design and synthesis of ultrathin catalysts.
The transferring and identification of single- and few- layer graphene sheets from SiO2/Si substrates to other types of substrates is presented. Features across large areas (∼cm2) having single and ...few-layer graphene flakes, obtained by the microcleaving of highly oriented pyrolytic graphite (HOPG), can be transferred reliably. This method enables the fast localization of graphene sheets on substrates on which optical microscopy does not allow direct and fast visualization of the thin graphene sheets. No major morphological deformations, corrugations, or defects are induced on the graphene films when transferred to the target surface. Moreover, the differentiation between single and bilayer graphene via the G′ (∼2700 cm−1) Raman peak is demonstrated on various substrates. This approach opens up possibilities for the fabrication of graphene devices on a substrate material other than SiO2/Si.
We report on the experimental and numerical investigations of dissipative rogue waves (DRWs) among noise-like pulses, in a thulium-doped fiber laser mode locked by a monolayer MoS 2 saturable ...absorber. By increasing the pumping power or weakening the effective cavity spectral filtering, the statistics distributions of the pulse events deviate from the Gaussian statistics to the L-shaped distributions with long tail, accompanied by the increase of the DRWs proportion. Our observations reveal the dissipat-ive nature of rogue waves in dissipative systems.
We investigated the atomic structures, Raman spectroscopic and electrical transport properties of individual graphene nanoribbons (GNRs, widths ∼10–30 nm) derived from sonochemical unzipping of ...multiwalled carbon nanotubes (MWNTs). Aberration-corrected transmission electron microscopy (TEM) revealed a high percentage of two-layer (2 L) GNRs and some single-layer ribbons. The layer–layer stacking angles ranged from 0° to 30° including average chiral angles near 30° (armchair orientation) or 0° (zigzag orientation). A large fraction of GNRs with bent and smooth edges was observed, while the rest showed flat and less smooth edges (roughness ≤1 nm). Polarized Raman spectroscopy probed individual GNRs to reveal D/G ratios and ratios of D band intensities at parallel and perpendicular laser excitation polarization (D∥/D⊥). The observed spectroscopic trends were used to infer the average chiral angles and edge smoothness of GNRs. Electrical transport and Raman measurements were carried out for individual ribbons to correlate spectroscopic and electrical properties of GNRs.
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