Single- and few-layer crystals of exfoliated MoTe2 have been characterized spectroscopically by photoluminescence, Raman scattering, and optical absorption measurements. We find that MoTe2 in the ...monolayer limit displays strong photoluminescence. On the basis of complementary optical absorption results, we conclude that monolayer MoTe2 is a direct-gap semiconductor with an optical band gap of 1.10 eV. This new monolayer material extends the spectral range of atomically thin direct-gap materials from the visible to the near-infrared.
Rhenium disulfide (ReS2) is a semiconducting layered transition metal dichalcogenide that exhibits a stable distorted 1T phase. The reduced symmetry of this system leads to in-plane anisotropy in ...various material properties. Here, we demonstrate the strong anisotropy in the Raman scattering response for linearly polarized excitation. Polarized Raman scattering is shown to permit a determination of the crystallographic orientation of ReS2 through comparison with direct structural analysis by scanning transmission electron microscopy (STEM). Analysis of the frequency difference of appropriate Raman modes is also shown to provide a means of precisely determining layer thickness up to four layers.
Rhenium disulfide (ReS2), a layered group VII transition metal dichalcogenide, has been studied by optical spectroscopy. We demonstrate that the reduced crystal symmetry, as compared to the ...molybdenum and tungsten dichalcogenides, leads to anisotropic optical properties that persist from the bulk down to the monolayer limit. We find that the direct optical gap blueshifts from 1.47 eV in the bulk to 1.61 eV in the monolayer limit. In the ultrathin limit, we observe polarization-dependent absorption and polarized emission from the band-edge optical transitions. We thus establish ultrathin ReS2 as a birefringent material with strongly polarized direct optical transitions that vary in energy and orientation with sample thickness.
The electrical and thermal behavior of nanoscale devices based on two-dimensional (2D) materials is often limited by their contacts and interfaces. Here we report the temperature-dependent thermal ...boundary conductance (TBC) of monolayer MoS2 with AlN and SiO2, using Raman thermometry with laser-induced heating. The temperature-dependent optical absorption of the 2D material is crucial in such experiments, which we characterize here for the first time above room temperature. We obtain TBC ∼ 15 MW m–2 K–1 near room temperature, increasing as ∼ T 0.65 in the range 300−600 K. The similar TBC of MoS2 with the two substrates indicates that MoS2 is the “softer” material with weaker phonon irradiance, and the relatively low TBC signifies that such interfaces present a key bottleneck in energy dissipation from 2D devices. Our approach is needed to correctly perform Raman thermometry of 2D materials, and our findings are key for understanding energy coupling at the nanoscale.
Modulation of weak interlayer interactions between quasi-two-dimensional atomic planes in the transition metal dichalcogenides (TMDCs) provides avenues for tuning their functional properties. Here we ...show that above-gap optical excitation in the TMDCs leads to an unexpected large-amplitude, ultrafast compressive force between the two-dimensional layers, as probed by in situ measurements of the atomic layer spacing at femtosecond time resolution. We show that this compressive response arises from a dynamic modulation of the interlayer van der Waals interaction and that this represents the dominant light-induced stress at low excitation densities. A simple analytic model predicts the magnitude and carrier density dependence of the measured strains. This work establishes a new method for dynamic, nonequilibrium tuning of correlation-driven dispersive interactions and of the optomechanical functionality of TMDC quasi-two-dimensional materials.
Ultrafast electrically driven nanoscale light sources are critical components in nanophotonics. Compound semiconductor-based light sources for the nanophotonic platforms have been extensively ...investigated over the past decades. However, monolithic ultrafast light sources with a small footprint remain a challenge. Here, we demonstrate electrically driven ultrafast graphene light emitters that achieve light pulse generation with up to 10 GHz bandwidth across a broad spectral range from the visible to the near-infrared. The fast response results from ultrafast charge-carrier dynamics in graphene and weak electron-acoustic phonon-mediated coupling between the electronic and lattice degrees of freedom. We also find that encapsulating graphene with hexagonal boron nitride (hBN) layers strongly modifies the emission spectrum by changing the local optical density of states, thus providing up to 460% enhancement compared to the gray-body thermal radiation for a broad peak centered at 720 nm. Furthermore, the hBN encapsulation layers permit stable and bright visible thermal radiation with electronic temperatures up to 2000 K under ambient conditions as well as efficient ultrafast electronic cooling via near-field coupling to hybrid polaritonic modes under electrical excitation. These high-speed graphene light emitters provide a promising path for on-chip light sources for optical communications and other optoelectronic applications.
Understanding growth, grain boundaries (GBs), and defects of emerging two-dimensional (2D) materials is key to enabling their future applications. For quick, nondestructive metrology, many studies ...rely on confocal Raman spectroscopy, the spatial resolution of which is constrained by the diffraction limit (∼0.5 μm). Here we use tip-enhanced Raman spectroscopy (TERS) for the first time on synthetic MoSe2 monolayers, combining it with other scanning probe microscopy (SPM) techniques, all with sub-20 nm spatial resolution. We uncover strong nanoscale heterogeneities in the Raman spectra of MoSe2 transferred to gold substrates one near 240 cm–1 (A1′), and others near 287 cm–1 (E′), 340 cm–1, and 995 cm–1, which are not observable with common confocal techniques and appear to imply the presence of nanoscale domains of MoO3. We also observe strong tip-enhanced photoluminescence (TEPL), with a signal nearly an order of magnitude greater than the far-field PL. Combining TERS with other SPM techniques, we find that GBs can cut into larger domains of MoSe2, and that carrier densities are higher at GBs than away from them.
Ultrathin transition metal dichalcogenides (TMDCs) have recently been extensively investigated to understand their electronic and optical properties. Here we study ultrathin Mo0.91W0.09Te2, a ...semiconducting alloy of MoTe2, using Raman, photoluminescence (PL), and optical absorption spectroscopy. Mo0.91W0.09Te2 transitions from an indirect to a direct optical band gap in the limit of monolayer thickness, exhibiting an optical gap of 1.10 eV, very close to its MoTe2 counterpart. We apply tensile strain, for the first time, to monolayer MoTe2 and Mo0.91W0.09Te2 to tune the band structure of these materials; we observe that their optical band gaps decrease by 70 meV at 2.3% uniaxial strain. The spectral widths of the PL peaks decrease with increasing strain, which we attribute to weaker exciton–phonon intervalley scattering. Furthermore, strained MoTe2 and Mo0.91W0.09Te2 extend the range of band gaps of TMDC monolayers further into the near-infrared, an important attribute for potential applications in optoelectronics.
Many web-based attacks have been studied to understand how web hackers behave, but web site defacement attacks (malicious content manipulations of victim web sites) and defacers' behaviors have ...received less attention from researchers. This paper fills this research gap via a computational data-driven analysis of a public database of defacers and defacement attacks and activities of 96 selected defacers who were active on Twitter. We conducted a comprehensive analysis of the data: an analysis of a friendship graph with 10,360 nodes, an analysis on how sentiments of defacers related to attack patterns, and a topical modelling based analysis to study what defacers discussed publicly on Twitter. Our analysis revealed a number of key findings: a modular and hierarchical clustering method can help discover interesting sub-communities of defacers; sentiment analysis can help categorize behaviors of defacers in terms of attack patterns; and topic modelling revealed some focus topics (politics, country-specific topics, and technical discussions) among defacers on Twitter and also geographic links of defacers sharing similar topics. We believe that these findings are useful for a better understanding of defacers' behaviors, which could help design and development of better solutions for detecting defacers and even preventing impeding defacement attacks.
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