Developments in optoelectronics and spin-optronics based on transition metal dichalcogenide monolayers (MLs) need materials with efficient optical emission and well-defined transition energies. In as-exfoliated MoS2 MLs the photoluminescence (PL) spectra even at low temperature consists typically of broad, overlapping contributions from neutral, charged excitons (trions) and localized states. Here we show that in superacid treated MoS2 MLs the PL intensity increases by up to 60 times at room temperature. The neutral and charged exciton transitions are spectrally well separated in PL and reflectivity at T = 4 K, with linewidth for the neutral exciton of 15 meV, but with similar intensities compared to the ones in as-exfoliated MLs at the same temperature. Time resolved experiments uncover picoseconds recombination dynamics analyzed separately for charged and neutral exciton emission. Using the chiral interband selection rules, we demonstrate optically induced valley polarization for both complexes and valley coherence for only the neutral exciton.Introduction.-Transition metal dichalcogenide (TMD) monolayers (ML) such as MoS 2 , MoSe 2 , WS 2 and WSe 2 are a new class of two-dimensional semiconductors with a direct bandgap in the visible region of the spectrum [1-3] and very unique properties. Strong spin orbit coupling combined with a crystal lattice that has no inversion symmetry allows for optical manipulation of the spin and valley degree of freedom in these materials [4]. In addition to their potential for unconventional, atomically thin and flexible electronics or valleytronics, they also are ideal candidates for optoelectronic and spin-optronic applications. For example, solar cells
Van der Waals heterojunctions composed of graphene and transition metal dichalcogenides have gain much attention because of the possibility to control and tailor band structure, promising applications in two-dimensional optoelectronics and electronics. In this report, we characterized the van der Waals heterojunction MoSe/few-layer graphene with a high-quality interface using cutting-edge surface techniques scaling from atomic to microscopic range. These surface analyses gave us a complete picture of the atomic structure and electronic properties of the heterojunction. In particular, we found two important results: the commensurability between the MoSe and few-layer graphene lattices and a band-gap opening in the few-layer graphene. The band gap is as large as 250 meV, and we ascribed it to an interface charge transfer that results in an electronic depletion in the few-layer graphene. This conclusion is well supported by electron spectroscopy data and density functional theory calculations. The commensurability between the MoSe and graphene lattices as well as the band-gap opening clearly show that the interlayer interaction goes beyond the simple van der Waals interaction. Hence, stacking two-dimensional materials in van der Waals heterojunctions enables us to tailor the atomic and electronic properties of individual layers. It also permits the introduction of a band gap in few-layer graphene by interface charge transfer.
Janus single-layer transition metal dichalcogenides, in which the two chalcogen layers have a different chemical nature, push chemical composition control beyond what is usually achievable with van der Waals heterostructures. Here, we report such a Janus compound, SPtSe, which is predicted to exhibit strong Rashba spin–orbit coupling. We synthetized it by conversion of a single-layer of PtSe2 on Pt(111) via sulfurization under H2S atmosphere. Our in situ and operando structural analysis with grazing incidence synchrotron X-ray diffraction reveals the process by which the Janus alloy forms. The crystalline long-range order of the as-grown PtSe2 monolayer is first lost due to thermal annealing. A subsequent recrystallization in presence of a source of sulfur yields a highly ordered SPtSe alloy, which is isostructural to the pristine PtSe2. The chemical composition is resolved, layer-by-layer, using angle-resolved X-ray photoelectron spectroscopy, demonstrating that Se-by-S substitution occurs selectively in the topmost chalcogen layer.
The magnetic order associated with the degree of freedom of spin in two-dimensional (2D) materials is subjected to intense investigation because of its potential application in 2D spintronics and valley-related magnetic phenomena. We report here a bottom-up strategy using molecular beam epitaxy to grow and dope large-area (cm 2 ) few-layer MoSe 2 with Mn as a magnetic dopant.High-quality Mn-doped MoSe 2 layers are obtained for Mn content of less than 5 % (atomic). When increasing the Mn content above 5% we observe a clear transition from layer-by-layer to cluster growth. Magnetic measurements involving a transfer process of the cm 2 -large doped layers on 100micron-thick silicon substrate, show plausible proof of high-temperature ferromagnetism of 1 % and 10 % Mn-doped MoSe 2 . Although we could not point to a correlation between magnetic and electrical properties, we demonstrate that the transfer process described in this report permits to achieve conventional electrical and magnetic measurements on the doped layers transferred on any substrate. Therefore, this study provides a promising route to characterize stable ferromagnetic 2D layers, which is broadening the current start-of-the-art of 2D materials-based applications. * These authors contributed equally to this work. 1 arXiv:1906.04801v1 [cond-mat.mtrl-sci]
An electrodynamic containment system has been used to study the freeezing behaviour of supercooled water drops, of radius range 25 to 90 μm. The drops were freozen at temperatures between 0 and — 29°C in an environment whose relative humidity was approximately 90% with respect to ice. Freezing events were observed visually and photographically, and measurements were mager of the accompanying freactional mass loss Δm/m. The most common moger of freeezing (70% of the drops studied) resulted in an apparently spherical ice particle. However, 18% exhibited spikes or other protuberances and the freeezing of 3% was accompanied by the ejection of numerous ice particles. In each of these situations values of Δm/m ranged freom about 5 to 15%. A further 9% of the drops exhibited one or more secondary mass-loss events, occurring several seconds after the freeezing process was complete; these were thus indicative of the ejection of ice particles. Almost all of the values of Δm/m were significantly in excess of those predicted on the basis of evaporation during freeezing, suggesting that an additional mechanism of mass loss was also present. The measured freeezing times were consigerrably shorter than the classical values—at least, for the larger drops freeezing at warmer temperatures. Some visual observations were consistent with the “supersaturation wave” around a freeezing drop, which has been predicted by Nix and Fukuta (1974).
The introduction of magnetism in two-dimensional (2D) materials represents an intense field of research nowadays and the quest to reach above-room-temperature ordering temperatures is still underway. Intrinsic ferromagnetism was discovered in 2017 in CrI 3 and Cr 2 Ge 2 Te 6 in the monolayer form with low Curie temperatures. An alternative method to introduce magnetism into conventional 2D materials is substitutional doping with magnetic impurities similarly to three-dimensional diluted magnetic semiconductors. The case of Mn-doped transition metal dichalcogenide (MoS 2 , MoSe 2 , WS 2 , WSe 2 ) monolayers is very interesting because combining out-of-plane ferromagnetism and valley contrast leads to ferrovalley materials. In this work, we focus on the incorporation of Mn in MoSe 2 by molecular beam epitaxy on graphene which has been rarely addressed up to now. By using a multiscale characterization approach, we demonstrate that Mn atoms are incorporated into the MoSe 2 monolayer up to 5 atomic percent. However, when incorporated into the film, Mn atoms tend to diffuse to the grain edges forming undefined Mo x Mn y Se z phase at grain boundaries after completion of the MoSe 2 monolayer. This segregation leaves the crystalline and electronic structure of MoSe 2 unmodified. Above 5%, the saturation of Mn content in MoSe 2 leads to the formation of epitaxial MnSe clusters.
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