A decade of intense research on two-dimensional (2D) atomic crystals has revealed that their properties can differ greatly from those of the parent compound. These differences are governed by changes in the band structure due to quantum confinement and are most profound if the underlying lattice symmetry changes. Here we report a high-quality 2D electron gas in few-layer InSe encapsulated in hexagonal boron nitride under an inert atmosphere. Carrier mobilities are found to exceed 10 cm V s and 10 cm V s at room and liquid-helium temperatures, respectively, allowing the observation of the fully developed quantum Hall effect. The conduction electrons occupy a single 2D subband and have a small effective mass. Photoluminescence spectroscopy reveals that the bandgap increases by more than 0.5 eV with decreasing the thickness from bulk to bilayer InSe. The band-edge optical response vanishes in monolayer InSe, which is attributed to the monolayer's mirror-plane symmetry. Encapsulated 2D InSe expands the family of graphene-like semiconductors and, in terms of quality, is competitive with atomically thin dichalcogenides and black phosphorus.
Strong quantization effects and tuneable near‐infrared photoluminescence emission are reported in mechanically exfoliated crystals of γ‐rhombohedral semiconducting InSe. The optical properties of InSe nanosheets differ qualitatively from those reported recently for exfoliated transition metal dichalcogenides and indicate a crossover from a direct to an indirect band gap semiconductor when the InSe flake thickness is reduced to a few nanometers.
High broad‐band photoresponsivity of mechanically formed InSe–graphene van der Waals heterostructures is achieved by exploiting the broad‐band transparency of graphene, the direct bandgap of InSe, and the favorable band line up of InSe with graphene. The photoresponsivity exceeds that for other van der Waals heterostructures and the spectral response extends from the near‐infrared to the visible spectrum.
Understanding how complex systems respond to change is of fundamental importance in the natural sciences. There is particular interest in systems whose classical newtonian motion becomes chaotic as an applied perturbation grows. The transition to chaos usually occurs by the gradual destruction of stable orbits in parameter space, in accordance with the Kolmogorov-Arnold-Moser (KAM) theorem--a cornerstone of nonlinear dynamics that explains, for example, gaps in the asteroid belt. By contrast, 'non-KAM' chaos switches on and off abruptly at critical values of the perturbation frequency. This type of dynamics has wide-ranging implications in the theory of plasma physics, tokamak fusion, turbulence, ion traps, and quasicrystals. Here we realize non-KAM chaos experimentally by exploiting the quantum properties of electrons in the periodic potential of a semiconductor superlattice with an applied voltage and magnetic field. The onset of chaos at discrete voltages is observed as a large increase in the current flow due to the creation of unbound electron orbits, which propagate through intricate web patterns in phase space. Non-KAM chaos therefore provides a mechanism for controlling the electrical conductivity of a condensed matter device: its extreme sensitivity could find applications in quantum electronics and photonics.
We present an overview of the main techniques for production and processing of graphene and related materials (GRMs), as well as the key characterization procedures. We adopt a ‘hands-on’ approach, providing practical details and procedures as derived from literature as well as from the authors’ experience, in order to enable the reader to reproduce the results. Section is devoted to ‘bottom up’ approaches, whereby individual constituents are pieced together into more complex structures. We consider graphene nanoribbons (GNRs) produced either by solution processing or by on-surface synthesis in ultra high vacuum (UHV), as well carbon nanomembranes (CNM). Production of a variety of GNRs with tailored band gaps and edge shapes is now possible. CNMs can be tuned in terms of porosity, crystallinity and electronic behaviour. Section covers ‘top down’ techniques. These rely on breaking down of a layered precursor, in the graphene case usually natural crystals like graphite or artificially synthesized materials, such as highly oriented pyrolythic graphite, monolayers or few layers (FL) flakes. The main focus of this section is on various exfoliation techniques in a liquid media, either intercalation or liquid phase exfoliation (LPE). The choice of precursor, exfoliation method, medium as well as the control of parameters such as time or temperature are crucial. A definite choice of parameters and conditions yields a particular material with specific properties that makes it more suitable for a targeted application. We cover protocols for the graphitic precursors to graphene oxide (GO). This is an important material for a range of applications in biomedicine, energy storage, nanocomposites, etc. Hummers’ and modified Hummers’ methods are used to make GO that subsequently can be reduced to obtain reduced graphene oxide (RGO) with a variety of strategies. GO flakes are also employed to prepare three-dimensional (3d) low density structures, such as sponges, foams, hydro- or aerogels. The assembly of flakes into 3d structures can provide improved mechanical properties. Aerogels with a highly open structure, with interconnected hierarchical pores, can enhance the accessibility to the whole surface area, as relevant for a number of applications, such as energy storage. The main recipes to yield graphite intercalation compounds (GICs) are also discussed. GICs are suitable precursors for covalent functionalization of graphene, but can also be used for the synthesis of uncharged graphene in solution. Degradation of the molecules intercalated in GICs can be triggered by high temperature treatment or microwave irradiation, creating a gas pressure surge in graphite and exfoliation. Electrochemical exfoliation by applying a voltage in an electrolyte to a graphite electrode can be tuned by varying precursors, electrolytes and potential. Graphite electrodes can be either negatively or positively intercalated to obtain GICs that are subsequently exfoliated. We also discuss the materials that can be amenable to exfoliation, by ...
The integration of different two-dimensional materials within a multilayer van der Waals (vdW) heterostructure offers a promising technology for high performance opto-electronic devices such as photodetectors and light sources. Here we report on the fabrication and electronic properties of vdW heterojunction diodes composed of the direct band gap layered semiconductors InSe and GaSe and transparent monolayer graphene electrodes. We show that the type II band alignment between the two layered materials and their distinctive spectral response, combined with the short channel length and low electrical resistance of graphene electrodes, enable efficient generation and extraction of photoexcited carriers from the heterostructure even when no external voltage is applied. Our devices are fast (∼2 μs), self-driven photodetectors with multicolor photoresponse ranging from the ultraviolet to the near-infrared and offer new routes to miniaturized optoelectronics beyond present semiconductor materials and technologies.
The electronic band structure of van der Waals (vdW) layered crystals has properties that depend on the composition, thickness and stacking of the component layers. Here we use density functional theory and high field magneto-optics to investigate the metal chalcogenide InSe, a recent addition to the family of vdW layered crystals, which transforms from a direct to an indirect band gap semiconductor as the number of layers is reduced. We investigate this direct-to-indirect bandgap crossover, demonstrate a highly tuneable optical response from the near infrared to the visible spectrum with decreasing layer thickness down to 2 layers, and report quantum dot-like optical emissions distributed over a wide range of energy. Our analysis also indicates that electron and exciton effective masses are weakly dependent on the layer thickness and are significantly smaller than in other vdW crystals. These properties are unprecedented within the large family of vdW crystals and demonstrate the potential of InSe for electronic and photonic technologies.
Van der Waals (vdW) interfaces based on two dimensional (2D) materials are promising for optoelectronics, as interlayer transitions between different compounds allow tailoring the spectral response over a broad range. However, issues such as lattice mismatch or a small misalignment of the constituent layers can drastically suppress electron-photon coupling for these interlayer transitions.Here, we engineer type-II interfaces by assembling atomically thin crystals that have the bottom of the conduction band and the top of the valence band at the Γ-point, thus avoiding any momentum mismatch. We find that these vdW interfaces exhibit radiative optical transitions irrespective of lattice constant, rotational/translational alignment of the two layers, or whether the constituent materials are direct or indirect gap semiconductors. Being robust and of general validity, our results broaden the scope of future optoelectronics device applications based on two-dimensional materials. Van der Waals interfaces of interest for optoelectronics consist of two distinct layered semiconductors with a suitable energetic alignment of their conduction and valence bands, such that electron and hole excitations reside in the two separate layers.[1-4] This allows the interfacial band gap to be controlled by material selection -as well as by application of an electrical bias or strain[5-9]-so that electron-hole recombination across the layers generates photons with frequency determined over a broad range at the design stage. Choosing the interface components among the vast gamut of 2D materials -including semiconducting transition metal dichalcogenides (TMDs, MoS 2 , MoSe 2 , MoTe 2 , WS 2 , WSe 2 , ReS 2 , ZrS 2 , etc.), III-VI compounds (InSe, GaSe), black phosphorous, and even magnetic semiconductors (CrI 3 , CrCl 3 , CrBr 3 , etc.)-enables, at least in principle, to cover a spectral range from the far infra-red to the violet. In practice, however, efficient light-emission from interlayer recombination requires the corresponding electron-hole transition to be direct in reciprocal (k-) space: the bottom of the conduction band in one layer has to be centered in k-space at the same position as the top of the valence band in the other layer.[10] This requirement poses severe constraints as concluded from heterostructures of monolayer semi-conducting TMDs, the systems that have been so far mostly used to realize light-emitting vdW interfaces. [7,[11][12][13][14] Indeed, in this case the minimum of the conduction band and top of valence band are at the K/K' points in the Brillouin zone and the presence of radiative
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