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Register a new userOptical control of charged exciton states in tungsten disulfide
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A method is presented for optically preparing WS2 monolayers to luminesce from only the charged exciton (trion) state--completely suppressing the neutral exciton. When isolating the trion state, we observed changes in the Raman A1g intensity and an enhanced feature on the low energy side of the E12g peak. Photoluminescence and optical reflectivity measurements confirm the existence of the prepared trion state. This technique also prepares intermediate regimes with controlled luminescence amplitudes of the neutral and charged exciton. This effect is reversible by exposing the sample to air, indicating the change is mitigated by surface interactions with the ambient environment. This method provides a tool to modify optical emission energy and to isolate physical processes in this and other two-dimensional materials.
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The ultrathin transition metal dichalcogenides (TMDs) have emerged as promising materials for various applications using two dimensional (2D) semiconductors. They have attracted increasing attention due to their unique optical properties originate from neutral and charged excitons. Here, we report negatively charged exciton formation in monolayer TMDs, notably tungsten disulfide WS2. Our theory is based on an effective mass model of neutral and charged excitons, parameterized by ab-initio calculations. Taking into the account the strong correlation between the monolayer WS2 and the surrounding dielectric environment, our theoretical results are in good agreement with one-photon photoluminescence (PL) and reflectivity measurements. We also show that the exciton state with p-symmetry, experimentally observed by two-photon PL emission, is energetically below the 2s-state. We use the equilibrium mass action law, to quantify the relative weight of exciton and trion PL. We show that exciton and trion emission can be tuned and controlled by external parameters like temperature, pumping and injection electrons. Finally, in comparison with experimental measurements, we show that exciton emission in monolayer tungsten dichalcogenides is substantially reduced. This feature suggests that free exciton can be trapped in disordered potential wells to form a localized exciton and therefore offers a route toward novel optical properties.
Raman scattering and photoluminescence (PL) emission are used to investigate a single layer of tungsten disulfide (WS$_{2}$) obtained by exfoliating n-type bulk crystals. Direct gap emission with both neutral and charged exciton recombination is observed in the low temperature PL spectra. The ratio between the trion and exciton emission can be tuned simply by varying the excitation power. Moreover, the intensity of the trion emission can be independently tuned using additional sub band gap laser excitation.
Dilute magnetic semiconductors, achieved through substitutional doping of spin-polarized transition metals into semiconducting systems, enable experimental modulation of spin dynamics in ways that hold great promise for novel magneto-electric or magneto-optical devices, especially for two-dimensional systems such as transition metal dichalcogenides that accentuate interactions and activate valley degrees of freedom. Practical applications of 2D magnetism will likely require room-temperature operation, air stability, and (for magnetic semiconductors) the ability to achieve optimal doping levels without dopant aggregation. Here we describe room-temperature ferromagnetic order obtained in semiconducting vanadium-doped tungsten disulfide monolayers produced by a reliable single-step film sulfidation method across an exceptionally wide range of vanadium concentrations, up to 12 at% with minimal dopant aggregation. These monolayers develop p-type transport as a function of vanadium incorporation and rapidly reach ambipolarity. Ferromagnetism peaks at an intermediate vanadium concentration of a few atomic percent and decreases for higher concentrations, which is consistent with quenching due to orbital hybridization at closer vanadium-vanadium spacings, as supported by transmission electron microscopy, magnetometry and first-principles calculations. Room-temperature two-dimensional dilute magnetic semiconductors provide a new component to expand the functional scope of van der Waals heterostructures and bring semiconducting magnetic 2D heterostructures them into the realm of practical application.
We present a complete characterisation at the nanoscale of the growth and structure of single-layer tungsten disulfide (WS$_2$) epitaxially grown on Au(111). Following the growth process in real time with fast x-ray photoelectron spectroscopy, we obtain a singly-oriented layer by choosing the proper W evaporation rate and substrate temperature during the growth. Information about the morphology, size and layer stacking of the WS$_2$ layer were achieved by employing x-ray photoelectron diffraction and low-energy electron microscopy. The strong spin splitting in the valence band of WS$_2$ coupled with the single-orientation character of the layer make this material the ideal candidate for the exploitation of the spin and valley degrees of freedom.
Porous single layer molybdenum disulfide (MoS$_2$) is a promising material for applications such as DNA sequencing and water desalination. In this work, we introduce irradiation with highly charged ions (HCIs) as a new technique to fabricate well-defined pores in MoS$_2$. Surprisingly, we find a linear increase of the pore creation efficiency over a broad range of potential energies. Comparison to atomistic simulations reveals the critical role of energy deposition from the ion to the material through electronic excitation in the defect creation process, and suggests an enrichment in molybdenum in the vicinity of the pore edges at least for ions with low potential energies. Analysis of the irradiated samples with atomic resolution scanning transmission electron microscopy reveals a clear dependence of the pore size on the potential energy of the projectiles, establishing irradiation with highly charged ions as an effective method to create pores with narrow size distributions and radii between ca. 0.3 and 3 nm.
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