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Register a new userIndirect to direct band gap crossover in two-dimensional WS2(1-x)Se2x alloys
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In atomically thin transition metal dichalcogenide semiconductors, there is a crossover from indirect to direct bandgap as the thickness drops to one monolayer, which comes with a fast increase of the photoluminescence signal. Here, we show that for different alloy compositions of WS2(1-x)Se2x this trend may be significantly affected by the alloy content and we demonstrate that the sample with the highest Se ratio presents a strongly reduced effect. The highest micro-PL intensity is found for bilayer WS2(1-x)Se2x (x = 0.8) with a decrease of its maximum value by only a factor of 2 when passing from mono- to bi-layer. To better understand this factor and explore the layer-dependent band structure evolution of WS2(1-x)Se2x, we performed a nano-angle resolved photoemission spectroscopy study coupled with first-principles calculations. We find that the high micro-PL value for bilayer WS2(1-x)Se2x (x = 0.8) is due to the overlay of direct and indirect optical transitions. This peculiar high PL intensity in WS2(1-x)Se2x opens the way for spectrally tunable light-emitting devices.
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Atomically thin films of III-VI post-transition metal chalcogenides (InSe and GaSe) form an interesting class of two-dimensional semiconductor that feature strong variations of their band gap as a function of the number of layers in the crystal [1-4] and, specifically for InSe, an earlier predicted crossover from a direct gap in the bulk [5,6] to a weakly indirect band gap in monolayers and bilayers [7-11]. Here, we apply angle resolved photoemission spectroscopy with submicrometer spatial resolution ($mu$ARPES) to visualise the layer-dependent valence band structure of mechanically exfoliated crystals of InSe. We show that for 1 layer and 2 layer InSe the valence band maxima are away from the $mathbf{Gamma}$-point, forming an indirect gap, with the conduction band edge known to be at the $mathbf{Gamma}$-point. In contrast, for six or more layers the bandgap becomes direct, in good agreement with theoretical predictions. The high-quality monolayer and bilayer samples enables us to resolve, in the photoluminescence spectra, the band-edge exciton (A) from the exciton (B) involving holes in a pair of deeper valence bands, degenerate at $mathbf{Gamma}$, with the splitting that agrees with both $mu$ARPES data and the results of DFT modelling. Due to the difference in symmetry between these two valence bands, light emitted by the A-exciton should be predominantly polarised perpendicular to the plane of the two-dimensional crystal, which we have verified for few-layer InSe crystals.
Alloying enables engineering of the electronic structure of semiconductors for optoelectronic applications. Due to their similar lattice parameters, the two-dimensional semiconducting transition metal dichalcogenides of the MoWSeS group (MX2 where M= Mo or W and X=S or Se) can be grown as high-quality materials with low defect concentrations. Here we investigate the atomic and electronic structure of Mo(1-x)WxS2 alloys using a combination of high-resolution experimental techniques and simulations. Analysis of the Mo and W atomic positions in these alloys, grown by chemical vapour transport, shows that they are randomly distributed, consistent with Monte Carlo simulations that use interaction energies determined from first-principles calculations. Electronic structure parameters are directly determined from angle resolved photoemission spectroscopy measurements. These show that the spin-orbit splitting at the valence band edge increases linearly with W content from MoS2 to WS2, in agreement with linear-scaling density functional theory (LS-DFT) predictions. The spin-orbit splitting at the conduction band edge is predicted to reduce to zero at intermediate compositions. Despite this, polarisation-resolved photoluminescence spectra on monolayer Mo0.5W0.5S2 show significant circular dichroism, indicating that spin-valley locking is retained. These results demonstrate that alloying is an important tool for controlling the electronic structure of MX2 for spintronic and valleytronic applications.
Two-dimensional transition-metal dichalcogendes $MX_2$ (es. MoS$_2$, WS$_2$, MoSe$_2$, ldots) are among the most promising materials for bandgap engineering. Widely studied in these compounds, by means of ab-initio techniques, is the possibility of tuning the direct-indirect gap character by means of in-plane strain. In such kind of calculations however the lattice degrees of freedom are assumed to be classical and frozen. In this paper we investigate in details the dependence of the bandgap character (direct vs. indirect) on the out-of-plane distance $h$ between the two chalcogen planes in each $MX_2$ unit. Using DFT calculations, we show that the bandgap character is indeed highly sensitive on the parameter $h$, in monolayer as well as in bilayer and bulk compounds, permitting for instance the switching from indirect to direct gap and from indirect to direct gap in monolayer systems. This scenario is furthermore analyzed in the presence of quantum lattice fluctuation induced by the zero-point motion. On the basis of a quantum analysis, we argue that the direct-indirect bandgap transitions induced by the out-of-plane strain as well by the in-plane strain can be regarded more as continuous crossovers rather than as real sharp transitions. The consequences on the physical observables are discussed.
Graphene and other two-dimensional materials display remarkable optical properties, including a simple light transparency of $T approx 1 - pi alpha$ for light in the visible region. Most theoretical rationalizations of this universal opacity employ a model coupling light to the electrons crystal momentum and put emphasis on the linear dispersion of the graphene bands. However, such a formulation of interband absorption is not allowable within band structure theory, because it conflates the crystal momentum label with the canonical momentum operator. We show that the physical origin of the optical behavior of graphene can be explained within a straightforward picture with the correct use of canonical momentum coupling. Its essence lies in the two-dimensional character of the density of states rather than in the precise dispersion relation, and therefore the discussion is applicable to other systems such as semiconductor membranes. At higher energies the calculation predicts a peak corresponding to a van Hove singularity as well as a specific asymmetry in the absorption spectrum of graphene, in agreement with previous results.
Quantum materials that host a flat band, such as pseudospin-1 lattices and magic-angle twisted bilayer graphene, can exhibit drastically new physical phenomena including unconventional superconductivity, orbital ferromagnetism, and Chern insulating behaviors. We report a surprising class of electronic in-gap edge states in pseudospin-1 materials without the conventional need of band-inversion topological phase transitions or introducing magnetism via an external magnetic type of interactions. In particular, we find that, in two-dimensional gapped (insulating) Dirac systems of massive spin-1 quasiparticles, in-gap edge modes can emerge through only an {em electrostatic potential} applied to a finite domain. Associated with these unconventional edge modes are spontaneous formation of pronounced domain-wall spin textures, which exhibit the feature of out-of-plane spin-angular momentum locking on both sides of the domain boundary and are quite robust against boundary deformations and impurities despite a lack of an explicit topological origin. The in-gap modes are formally three-component evanescent wave solutions, akin to the Jackiw-Rebbi type of bound states. Such modes belong to a distinct class due to the following physical reasons: three-component spinor wave function, unusual boundary conditions, and a shifted flat band induced by the external scalar potential. Not only is the finding of fundamental importance, but it also paves the way for generating highly controllable in-gap edge states with emergent spin textures using the traditional semiconductor gate technology. Results are validated using analytic calculations of a continuum Dirac-Weyl model and tight-binding simulations of realistic materials through characterizations of local density of state spectra and resonant tunneling conductance.
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