Van der Waals heterostructures have recently emerged as a new class of materials, where quantum coupling between stacked atomically thin two-dimensional layers, including graphene, hexagonal-boron nitride and transition-metal dichalcogenides (MX2), give rise to fascinating new phenomena. MX2 heterostructures are particularly exciting for novel optoelectronic and photovoltaic applications, because two-dimensional MX2 monolayers can have an optical bandgap in the near-infrared to visible spectral range and exhibit extremely strong light-matter interactions. Theory predicts that many stacked MX2 heterostructures form type II semiconductor heterojunctions that facilitate efficient electron-hole separation for light detection and harvesting. Here, we report the first experimental observation of ultrafast charge transfer in photoexcited MoS2/WS2 heterostructures using both photoluminescence mapping and femtosecond pump-probe spectroscopy. We show that hole transfer from the MoS2 layer to the WS2 layer takes place within 50 fs after optical excitation, a remarkable rate for van der Waals coupled two-dimensional layers. Such ultrafast charge transfer in van der Waals heterostructures can enable novel two-dimensional devices for optoelectronics and light harvesting.
Layered transition metal dichalcogenides (TMDs) draw much attention as the key semiconducting material for two-dimensional electrical, optoelectronic, and spintronic devices. For most of these applications, both n- and p-type materials are needed to form junctions and support bipolar carrier conduction. However, typically only one type of doping is stable for a particular TMD. For example, molybdenum disulfide (MoS2) is natively an n-type presumably due to omnipresent electron-donating sulfur vacancies, and stable/controllable p-type doping has not been achieved. The lack of p-type doping hampers the development of charge-splitting p-n junctions of MoS2, as well as limits carrier conduction to spin-degenerate conduction bands instead of the more interesting, spin-polarized valence bands. Traditionally, extrinsic p-type doping in TMDs has been approached with surface adsorption or intercalation of electron-accepting molecules. However, practically stable doping requires substitution of host atoms with dopants where the doping is secured by covalent bonding. In this work, we demonstrate stable p-type conduction in MoS2 by substitutional niobium (Nb) doping, leading to a degenerate hole density of ∼ 3 × 10(19) cm(-3). Structural and X-ray techniques reveal that the Nb atoms are indeed substitutionally incorporated into MoS2 by replacing the Mo cations in the host lattice. van der Waals p-n homojunctions based on vertically stacked MoS2 layers are fabricated, which enable gate-tunable current rectification. A wide range of microelectronic, optoelectronic, and spintronic devices can be envisioned from the demonstrated substitutional bipolar doping of MoS2. From the miscibility of dopants with the host, it is also expected that the synthesis technique demonstrated here can be generally extended to other TMDs for doping against their native unipolar propensity.
Elastic properties of materials are an important factor in their integration in applications. Chemical vapor deposited (CVD) monolayer semiconductors are proposed as key components in industrial-scale flexible devices and building blocks of two-dimensional (2D) van der Waals heterostructures. However, their mechanical and elastic properties have not been fully characterized. Here we report high 2D elastic moduli of CVD monolayer MoS2 and WS2 (∼170 N/m), which is very close to the value of exfoliated MoS2 monolayers and almost half the value of the strongest material, graphene. The 2D moduli of their bilayer heterostructures are lower than the sum of 2D modulus of each layer but comparable to the corresponding bilayer homostructure, implying similar interactions between the hetero monolayers as between homo monolayers. These results not only provide deep insight into understanding interlayer interactions in 2D van der Waals structures but also potentially allow engineering of their elastic properties as desired.
We report a simple and effective way of fabricating high-quality carbon nanoscrolls (CNSs), using isopropyl alcohol solution to roll up monolayer graphene predefined on SiO(2)/Si substrates. Transmission electron microscopy studies reveal that the CNS has a tube-like structure with a hollow core surrounded by graphene walls 0.35 nm apart. Raman spectroscopy studies show that the CNS is free of significant defects, and the electronic structure and phonon dispersion are slightly different from those of two-dimensional graphene. Finally, the CNS-based device is fabricated, directly on the SiO(2)/Si substrate. Electrical-transport measurements show that its resistance is weakly gate-dependent but strongly temperature-dependent. In addition, the CNS can sustain a high current density up to 5 x 10(7) A/cm(2), indicating that it is a good candidate for microcircuit interconnects. The controlled fabrication of high-quality CNSs may open up new opportunities for both fundamental and applied research of CNSs.
A straightforward roll‐to‐roll process for fabricating flexible and stretchable superaligned carbon nanotube films as transparent conducting films is demonstrated. Practical touch panels assembled by using these carbon nanotube conducting films are superior in flexibility and wearability—and comparable in linearity—to touch panels based on indium tin oxide (ITO) films. After suitable laser trimming and deposition of Ni and Au metal, the carbon nanotube film possesses excellent performance with two typical values of sheet resistances and transmittances (208 Ω □−1, 90% and 24 Ω □−1, 83.4%), which are comparable to ITO films and better than the present carbon nanotube conducting films in literature. The results provide a route to produce transparent conducting films more easily, effectively, and cheaply, an important step for realizing industrial‐scale applications of carbon nanotubes for transparent conducting films.
We report controlled syntheses of super-aligned carbon nanotube (CNT) arrays with the desired tube-diameter, number of walls, and length for spinning continuous unidirectional sheets to meet a variety of industrial demands. The tube-diameter distribution of super-aligned arrays is well controlled by varying the thicknesses of catalyst films, and the length of them is tuned by the growth time. Further investigation indicates that the physical properties of the unidirectional sheets, such as electrical transport, optical transmittance, and light emission properties, can be well tuned by the tube-diameter- and length-controlled growth. This work extends the understanding of the super-aligned CNT arrays and will be very helpful in developing further applications.
High-strength and conductive carbon nanotube (CNT) yarns are very attractive in many potential applications. However, there is a difficulty when simultaneously enhancing the strength and conductivity of CNT yarns. Adding some polymers into CNT yarns to enhance their strength will decrease their conductivity, while treating them in acid or coating them with metal nanoparticles to enhance their conductivity will reduce their strength. To overcome this difficulty, here we report a method to make high-strength and highly conductive CNT-based composite yarns by using a continuous superaligned CNT (SACNT) yarn as a conductive framework and then inserting polyvinyl alcohol (PVA) into the intertube spaces of the framework through PVA/dimethyl sulphoxide solution to enhance the strength of yarns. The as-produced CNT/PVA composite yarns possess very high tensile strengths up to 2.0 GPa and Young's moduli more than 120 GPa, much higher than those of the CNT/PVA yarns reported. The electric conductivity of as-produced composite yarns is as high as 9.2 × 10(4) S/m, comparable to HNO(3)-treated or Au nanoparticle-coated CNT yarns. These composite yarns are flexible, lightweight, scratch-resistant, very stable in the lab environment, and resistant to extremely humid ambient and as a result can be woven into high-strength and heatable fabrics, showing potential applications in flexible heaters, bullet-proof vests, radiation protection suits, and spacesuits.
Phonon polaritons are quasiparticles resulting from strong coupling of photons with optical phonons. Excitation and control of these quasiparticles in 2D materials offer the opportunity to confine and transport light at the nanoscale. Here, we image the phonon polariton (PhP) spectral response in thin hexagonal boron nitride (hBN) crystals as a representative 2D material using amplitude-and phase-resolved scattering scanning near-field optical microscopy (s-SNOM) using broadband mid-IR synchrotron radiation. The large spectral bandwidth enables the simultaneous measurement of both out-of-plane (780 cm −1 ) and in-plane (1370 cm −1 ) hBN phonon modes. In contrast to the strong in-plane mode, the out-of-plane PhP mode response is weak. Measurements of the PhP wavelength reveal a proportional dependence on sample thickness for thin hBN flakes, which can be understood by a general model describing two-dimensional polariton excitation in ultrathin materials. KEYWORDS: phonon polariton, boron nitride, near-field spectroscopy, synchrotron infrared nanospectroscopy (SINS) P honon polaritons 1 (PhPs) result from coupling of photons with optical phonons in polar crystals. Unlike plasmon polaritons, 2−4 which usually span a very broad energy range, PhPs provide a spectrally selective response related to the optical phonon modes in the infrared to terahertz spectral range. The PhPs can have strong spatial confinement and may enable potential applications for enhanced IR light−matter interaction, 5,6 high-density IR data storage, 7 coherent thermal emission, 8 development of metamaterials, 9,10 and frequencytunable terahertz wave generation. 11 Hexagonal boron nitride (hBN) is a convenient model system for studying PhPs in ultrathin materials because hBN flakes with different thicknesses are easy to prepare with high quality and no dangling bonds as a two-dimensional (2D) van der Waals material. It has two Reststrahlen bands in the midinfrared region spanning the transverse (ω TO ) and longitudinal (ω LO ) phonon frequencies of the out-of-plane mode (ω TO = 760, ω LO = 825 cm −1 ) and the in-plane mode (ω TO = 1370, ω LO = 1614 cm −1 ). Both the lower frequency out-of-plane mode and the higher frequency in-plane mode have negative real parts of the dielectric function and thus have the potential to support PhPs. 12 Furthermore, hBN is a promising material for nanotechnology applications due to its 2D layered structure, excellent electrical insulation, and chemical and thermal stability. It has attracted great interest as a substrate for highmobility graphene, 13−17 as an ideal dielectric layer and spacer for 2D heterostructures, 18,19 and for its intrinsic UV lasing response. 20 Recently, the hBN PhP related behavior started to attract much interest. 21−24 Dai et al. studied PhPs in thin hBN flakes with laser-based scattering scanning near-field optical microscopy (s-SNOM) and observed a thickness-dependent PhP dispersion 21 in the upper spectral range around the in-plane (∼1370 cm −1 ) vibration phonon mode. However, they ...
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