The emergence of two-dimensional electronic materials has stimulated proposals of novel electronic and photonic devices based on the heterostructures of transition metal dichalcogenides. Here we ...report the determination of band offsets in the heterostructures of transition metal dichalcogenides by using microbeam X-ray photoelectron spectroscopy and scanning tunnelling microscopy/spectroscopy. We determine a type-II alignment between MoS2 and WSe2 with a valence band offset value of 0.83 eV and a conduction band offset of 0.76 eV. First-principles calculations show that in this heterostructure with dissimilar chalcogen atoms, the electronic structures of WSe2 and MoS2 are well retained in their respective layers due to a weak interlayer coupling. Moreover, a valence band offset of 0.94 eV is obtained from density functional theory, consistent with the experimental determination.
We present first-principles calculations of silicene/graphene and germanene/graphene bilayers. Various supercell models are constructed in the calculations in order to reduce the strain of the ...lattice-mismatched bilayer systems. Our energetics analysis and electronic structure results suggest that graphene can be used as a substrate to synthesize monolayer silicene and germanene. Multiple phases of single crystalline silicene and germanene with different orientations relative to the substrate could coexist at room temperature. The weak interaction between the overlayer and the substrate preserves the low-buckled structure of silicene and germanene, as well as their linear energy bands. The gap induced by breaking the sublattice symmetry in silicene on graphene can be up to 57 meV.
Due to its high carrier mobility, broadband absorption, and fast response time, the semi-metallic graphene is attractive for optoelectronics. Another two-dimensional semiconducting material ...molybdenum disulfide (MoS2) is also known as light- sensitive. Here we show that a large-area and continuous MoS2 monolayer is achievable using a CVD method and graphene is transferable onto MoS2. We demonstrate that a photodetector based on the graphene/MoS2 heterostructure is able to provide a high photogain greater than 10(8). Our experiments show that the electron-hole pairs are produced in the MoS2 layer after light absorption and subsequently separated across the layers. Contradictory to the expectation based on the conventional built-in electric field model for metal-semiconductor contacts, photoelectrons are injected into the graphene layer rather than trapped in MoS2 due to the presence of a perpendicular effective electric field caused by the combination of the built-in electric field, the applied electrostatic field, and charged impurities or adsorbates, resulting in a tuneable photoresponsivity.
Semiconductor heterostructures have played a critical role as the enabler for new science and technology. The emergence of transition‐metal dichalcogenides (TMDs) as atomically thin semiconductors ...has opened new frontiers in semiconductor heterostructures either by stacking different TMDs to form vertical heterojunctions or by stitching them laterally to form lateral heterojunctions via direct growth. In conventional semiconductor heterostructures, the design of multijunctions is critical to achieve carrier confinement. Analogously, successful synthesis of a monolayer WS2/WS2(1−x)Se2x/WS2 multijunction lateral heterostructure via direct growth by chemical vapor deposition is reported. The grown structures are characterized by Raman, photoluminescence, and annular dark‐field scanning transmission electron microscopy to determine their lateral compositional profile. More importantly, using microwave impedance microscopy, it is demonstrated that the local photoconductivity in the alloy region can be tailored and enhanced by two orders of magnitude over pure WS2. Finite element analysis confirms that this effect is due to the carrier diffusion and confinement into the alloy region. This work exemplifies the technological potential of atomically thin lateral heterostructures in optoelectronic applications.
The successful synthesis of a monolayer lateral heterostructure with multijunctions WS2/WS2(1−x)Se2x/WS2 (x ≈ 0.15) by chemical vapor deposition is reported. The grown structures are characterized by Raman and photoluminescence. Using light‐assisted microwave impedance microscopy, the multijunctions demonstrate that the local photoconductivity in the alloy region can be tailored and enhanced by two orders of magnitude over pure WS2.
Palladium diselenide (PdSe2), a peculiar noble metal dichalcogenide, has emerged as a new two-dimensional material with high predicted carrier mobility and a widely tunable band gap for device ...applications. The inherent in-plane anisotropy endowed by the pentagonal structure further renders PdSe2 promising for novel electronic, photonic, and thermoelectric applications. However, the direct synthesis of few-layer PdSe2 is still challenging and rarely reported. Here, we demonstrate that few-layer, single-crystal PdSe2 flakes can be synthesized at a relatively low growth temperature (300 °C) on sapphire substrates using low-pressure chemical vapor deposition (CVD). The well-defined rectangular domain shape and precisely determined layer number of the CVD-grown PdSe2 enable us to investigate their layer-dependent and in-plane anisotropic properties. The experimentally determined layer-dependent band gap shrinkage combined with first-principle calculations suggest that the interlayer interaction is weaker in few-layer PdSe2 in comparison with that in bulk crystals. Field-effect transistors based on the CVD-grown PdSe2 also show performances comparable to those based on exfoliated samples. The low-temperature synthesis method reported here provides a feasible approach to fabricate high-quality few-layer PdSe2 for device applications.
By using direct growth, we create a rotationally aligned MoS2/WSe2 hetero-bilayer as a designer van der Waals heterostructure. With rotational alignment, the lattice mismatch leads to a periodic ...variation of atomic registry between individual van der Waals layers, exhibiting a Moiré pattern with a well-defined periodicity. By combining scanning tunneling microscopy/spectroscopy, transmission electron microscopy, and first-principles calculations, we investigate interlayer coupling as a function of atomic registry. We quantitatively determine the influence of interlayer coupling on the electronic structure of the hetero-bilayer at different critical points. We show that the direct gap semiconductor concept is retained in the bilayer although the valence and conduction band edges are located at different layers. We further show that the local bandgap is periodically modulated in the X-Y direction with an amplitude of ~0.15 eV, leading to the formation of a two-dimensional electronic superlattice.
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