To date, quantum communication widely relies on attenuated lasers for secret key generation. In future quantum networks, fundamental limitations resulting from their probabilistic photon distribution must be overcome by using deterministic quantum light sources. Confined excitons in monolayers of transition metal dichalcogenides (TMDCs) constitute an emerging type of emitter for quantum light generation. These atomically thin solid-state sources show appealing prospects for large-scale and low-cost device integration, meeting the demands of quantum information technologies. Here, we pioneer the practical suitability of TMDC devices in quantum communication. We employ a WSe2 monolayer single-photon source to emulate the BB84 protocol in a quantum key distribution (QKD) setup and achieve click rates of up to 66.95 kHz and antibunching values down to 0.034—a performance competitive with QKD experiments using semiconductor quantum dots or color centers in diamond. Our work opens the route towards wider applications of quantum information technologies using TMDC single-photon sources.

Two-dimensional layered gallium monochalcogenide (GaX, where X = S, Se, Te) semiconductors possess great potential for use in optoelectronic and photonic applications, owing to their direct band edge. In this work, the structural and optical properties of full-series multilayer GaTe1−xSex for x = 0 to x = 1 are examined. The experimental results show that the whole series of GaTe1−xSex layers may contain one hexagonal (H) phase from GaTe to GaSe, whereas the monoclinic (M) phase predominates at 0 ≤ x ≤ 0.4. For x ≥ 0.5, the H-phase dominates the GaTe1−xSex series. The micro-photoluminescence (μPL) results indicate that the photon emission energy of M-phase GaTe1−xSex increases as the Se content increases from 1.652 eV (M-GaTe) to 1.779 eV (M-GaTe0.6Se0.4), whereas that of H-phase GaTe1−xSex decreases from 1.998 eV (H-GaSe) to 1.588 eV (H-GaTe) in the red to near-infrared (NIR) region. Micro-time-resolved photoluminescence (TRPL) and area-fluorescence lifetime mapping (AFLM) of the few-layer GaTe1−xSex series indicates that the decay lifetime of the band-edge emission of the M phase is faster than that of the H phase in the mixed alloys of layered GaTe1−xSex (0 ≤ x ≤ 0.4). On the other hand, for H-phase GaTe1−xSex, the decay lifetime of the band-edge emission also increases as the Se content increases, owing to the surface effect. The dark resistivity of GaTe1−xSex for 0.5 ≤ x ≤ 1 (i.e., predominantly H phase) is greater than that of the other instance of majority M-phase GaTe1−xSex for 0 ≤ x ≤ 0.4, owing to the larger bandgaps. The predominantly H phase GaTe1−xSex (0.5 ≤ x ≤ 1) also shows a greater photoconductive response under visible-light illumination because of the greater contribution from surface states. The superior light-emission and photodetection capability of the GaTe1−xSex multilayers (0 ≤ x ≤ 1) means that they can be used for future optoelectronic devices.

The discovery of twisted bilayer graphene with tunable superconductivity has diverted great focus at the world of twisted van der Waals heterostructures. Here we propose a paradigm for bilayer materials, where covalent bonding replaces the van der Waals interaction between the layers. On the example of germanene-stanene bilayer, we show that such systems demonstrate fascinating topological properties and manifest giant capacitance effects of the order of C = 102μ F as well as dipole-like charge densities of q = 1 − 2 × 10−4μ C cm−2, showing promise for 2D ferroelectricity. The observed unique behaviour is closely linked to transverse strain-induced buckling deformations at the bilayer/substrate interface. In alternative GeSn bilayer structures with low twist angles the strain distortions trigger rich topological defect physics. We propose that the GeSn bilayer topology may be switched locally by a substrate-strain-induced electric fields. We demonstrate an approach to fabricate covalent bilayer materials, holding vast possibilities to transform applications technologies across solar, energy and optoelectronic sectors.

Semiconducting two-dimensional materials with chemical formula MoSi2X4 (X = N, P, or As) are studied by means of atomistic ground- and excited-state first-principles simulations. Full-fledged quasi-particle bandstructures within the G0W0 approach substantially correct the electronic bandgaps previously obtained with hybrid-functional density functional theory and highlight the absence of lateral valleys close in energy to the conduction band minimum. By solving the Bethe–Salpeter equation, we show that the optical properties are dominated by strongly bound excitons with the absorbance and maximum short-circuit current densities of MoSi2P4 and MoSi2As4 comparable to those of transition metal dichalcogenides. Due to the presence of the outer SiX layers, the exciton binding energies are smaller than those generally found for transition metal dichalcogenides. Long radiative lifetimes of bright excitons, over 10 ns at room temperature for MoSi2As4, and the absence of band-nesting are very promising for application in efficient ultra-thin optoelectronic devices.

Large-scale two-dimensional (2D) moiré superlattices are driving a revolution in designer quantum materials. The electronic interactions in these superlattices, strongly dependent on the periodicity and symmetry of the moiré pattern, critically determine the emergent properties and phase diagrams. To date, the relative twist angle between two layers has been the primary tuning parameter for a given choice of constituent crystals. Here, we establish strain as a powerful mechanism to in situ modify the moiré periodicity and symmetry. We develop an analytically exact mathematical description for the moiré lattice under arbitrary in-plane heterostrain acting on any bilayer structure. We demonstrate the ability to fine-tune the moiré lattice near critical points, such as the magic angle in bilayer graphene, or fully reconfigure the moiré lattice symmetry beyond that imposed by the unstrained constituent crystals. Due to this unprecedented simultaneous control over the strength of electronic interactions and lattice symmetry, 2D heterostrain provides a powerful platform to engineer, tune, and probe strongly correlated moiré materials.

2D metal-organic frameworks (2D-MOFs) materials can be subjected to various modes of mechanical stresses and strains in a wide range of applications, for which their mechanical properties are critical to reach practical implementations. Despite the rapid developments focused on the preparation of ultrathin 2D-MOF materials, very little is known about their mechanical and degradation behavior. Here, we use the established 2D-MOF PdTCPP-Cu (NAFS-13) as model system, to introduce the Langmuir–Blodgett (LB) technique, combined with interfacial rheology, as a novel in situ method for direct determination of the in-plane Young’s modulus by simultaneously measuring the 2D shear and compression moduli of a 2D-MOF formed at the air-water interface. Furthermore, it can be used to evaluate mechanistic models describing the degradation kinetics of 2D MOFs. To provide a deeper understanding of the factors that determine the Young’s modulus observed in such a set up, we carried out nanoindentation measurements and molecular dynamics (MD) simulations based on classical force fields. This protocol allows us to gain mechanistic insights into the impact of structural defects, temperature, tensile and compression stress on the Young’s modulus of 2D MOFs.

Among quantum devices based on 2D materials, gate-defined quantum confined 1D channels are much less explored, especially in the high-mobility regime where many-body interactions play an important role. We present the results of measurements and theory of conductance quantization in a gate-defined one-dimensional channel in a single layer of transition metal dichalcogenide material WSe2. In the quasi-ballistic regime of our high-mobility sample, we report conductance quantization steps in units of e2/h for a wide range of carrier concentrations. Magnetic field measurements show that as the field is raised, higher conductance plateaus move to accurate quantized values and then shift to lower conductance values while the e2/h plateau remains locked. Based on microscopic atomistic tight-binding theory, we show that in this material, valley and spin degeneracies result in 2 e2/h conductance steps for noninteracting holes, suggesting that symmetry-breaking mechanisms such as valley polarization dominate the transport properties of such quantum structures.

The Hofstadter butterfly is one of the first and most fascinating examples of the fractal and self-similar quantum nature of free electrons in a lattice pierced by a perpendicular magnetic field. However, the direct experimental verification of this effect on single-layer materials is still missing as very strong and inaccessible magnetic fields are necessary. For this reason, its indirect experimental verification has only been realized in artificial periodic 2D systems, like moiré lattices. The only recently synthesized 2D covalent organic frameworks might circumvent this limitation: Due to their large pore structures, magnetic fields needed to detect most features of the Hofstadter butterfly are indeed accessible with today technology. This work opens the door to make this exotic and theoretical issue from the 70s measurable and might solve the quest for the experimental verification of the Hofstadter butterfly in single-layer materials. Moreover, the intrinsic hierarchy of different pore sizes in 2D covalent organic framework adds additional complexity and beauty to the original butterflies and leads to a direct accessible playground for new physical observations.

The performance of transistors based on two-dimensional (2D) materials is affected largely by the contact resistance due to high Schottky barriers at the metal-2D-material interface. In this work, we incorporate the effect of surrounding dielectrics and image-force barrier-lowering in calculating the resistance of Schottky edge-contacts between a metal and a transition-metal dichalcogenide (TMD) thin layer. The electrostatic potential is computed by solving the Poisson equation numerically. The transmission probability is computed using the Wentzel–Kramers–Brillouin (WKB) approximation using the full-band density of states obtained from density functional theory (DFT). The effect of the image force is obtained analytically using the Coulomb kernel of a point charge with boundary conditions appropriate to the geometry we have considered. We find that the image-force barrier-lowering (IFBL) in edge-contacts is determined mainly by the dielectric permittivity of the surrounding oxide. We find that low-κ surrounding dielectrics are crucial for obtaining low resistance monolayer-TMD edge-contacts. Our results show metal-to-n(p)-type MoS2 (WSe2) edge-contacts with SiO2 as top and bottom insulators, a doping concentration > 1 × 1013cm−2 and a metal work-function 4.6 eV) result in a contact resistance as low as 50 Ω ⋅ μm.

Very recently, it has been reported that mixed transition metal oxide (TMO)/MXene catalysts show improved performance over TMO only catalysts for the oxygen evolution reaction (OER). However, the reasoning behind this observation is unknown. In this work mixed Co(OH)2/Ti3C2Tx were prepared and characterized for the OER using ex situ and operando spectroscopy techniques in order to initiate the understanding of why mixed TMO/MXene materials show better performances compared to TMO only catalysts. This work shows that the improved electrocatalysis for the composite material compared to the TMO only catalyst is due to the presence of higher Co oxide oxidation states at lower OER overpotentials for the mixed TMO/MXene catalysts. Furthermore, the presence of the MXene allows for a more mechanically robust film during OER, making the film more stable. Finally, our results show that small amounts of MXene are more advantageous for the OER during long-term stability measurements, which is linked to the formation of TiO2. The sensitivity of MXene oxidation ultimately limits TMO/MXene composites under alkaline OER conditions, meaning mass fractions must be carefully considered when designing such a catalyst to minimize the residual TiO2 formed during its lifetime.

Metal contacts form one of the main limitations for the introduction of 2D materials in next-generation scaled devices. Through ab-initio simulation techniques, we shed light on the fundamental physics and screen several 2D and 3D top and side contact metals. Our findings highlight that a low semiconducting-metal contact resistance can be achieved. By selecting an appropriate 2D metal, we demonstrate both ohmic or small Schottky barrier top and side contacts. This leads to a contact resistance below 100 Ωμm and good device drive performance with currents in ON state up to 1400 μA/μm, i.e., reduced by a mere 25% compared to a reference with perfect ohmic contacts, provided a sufficiently high doping concentration of 1.8×1013 cm−2 is used. Additionally, we show that this doping concentration can be achieved through electrostatic doping with a gate. Finally, we perform a screening of possible 2D–3D top contacts. Finding an ohmic 2D–3D contact without a Schottky barrier has proven difficult, but it is shown that for the case of intermediate interaction strength and a limited Schottky barrier, contact resistances below 100 Ωμm can be achieved.

van der Waals solids are well known to host remarkable phase diagrams with competing phases, unusual energy transfer processes, and elusive states of matter. Among this class of materials, chalcogenides have emerged as the most flexible and relevant platforms for unraveling charge–structure–function relationships. In order to explore the properties of complex chalcogenides under external stimuli, we measured the far infrared spectroscopic response of CrSiTe3 under extreme pressure–temperature conditions. Analysis of the 368 cm−1 Si–Te stretching mode and the manner in which it is screened by the closure of the indirect gap reveals that the insulator–metal transition takes place immediately after the structural phase transition—once the mixed phase aspect of the lattice distortion is resolved. At the same time, the two-phase region associated with the structural transition widens with decreasing temperature, and the slope of the insulator–metal transition under pressure is consistent with increasing entropy. These trends completely revise the character of the temperature–pressure phase diagram as well as the relationship between the structural and insulator–metal transitions, leading to a critical nexus of activity that may hide a quantum critical point and allow superconductivity to emerge.

Multiferroic materials, showing simultaneous ferroelectric and ferromagnetic orders, are considered to be promising candidates for future data storage technology however, the multiferroic phenomenon in two-dimensional (2D) materials is rarely observed. We report a simple approach to observe frequency-dependent ferroelectricity and multiferroicity in 2D Ti3C2Tx MXene film at room-temperature. To study the frequency and poling effect on ferroelectricity, we performed electric polarization vs. electric field (P-E) measurement at different frequencies, measured under zero and non-zero static magnetic fields. The results not only indicate a clear frequency dependence of electric domains owing to varying time relaxation during reversal dynamic but also showed magnetic field control of electric polarization thus, confirmed the presence of strong magneto-electric (ME) coupling at room-temperature. The existence of ME coupling was attributed to the coupling between disordered electric dipoles with local spin moments as well reduced dielectric loss after heat-treatment. Moreover, the ferroelectric Ti3C2Tx MXene film was employed as an active layer within the resistive data storage device that showed a stable switching behavior along with improved on/off ratio in comparison to non-ferroelectric Ti3C2Tx active layer. The unique multiferroic behavior along with ferroelectric-tuned data storage devices reported here, will help understand the intrinsic nature of 2D materials and will advance the 2D ferroelectric data storage industry.

The presence of metal atoms at the edges of graphene nanoribbons (GNRs) opens new possibilities toward tailoring their physical properties. We present here formation and high-resolution characterization of indium (In) chains on the edges of graphene-supported GNRs. The GNRs are formed when adsorbed hydrocarbon contamination crystallizes via laser heating into small ribbon-like patches of a second graphitic layer on a continuous graphene monolayer and onto which In is subsequently physical vapor deposited. Using aberration-corrected scanning transmission electron microscopy (STEM), we find that this leads to the preferential decoration of the edges of the overlying GNRs with multiple In atoms along their graphitic edges. Electron-beam irradiation during STEM induces migration of In atoms along the edges of the GNRs and triggers the formation of longer In atom chains during imaging. Density functional theory (DFT) calculations of GNRs similar to our experimentally observed structures indicate that both bare zigzag (ZZ) GNRs as well as In-terminated ZZ-GNRs have metallic character, whereas in contrast, In termination induces metallicity for otherwise semiconducting armchair (AC) GNRs. Our findings provide insights into the creation and properties of long linear metal atom chains at graphitic edges.

The discovery of two-dimensional (2D) van der Waals (vdW) materials often provides interesting playgrounds to explore novel phenomena. One of the missing components in 2D vdW materials is the intrinsic heavy-fermion systems, which can provide an additional degree of freedom to study quantum critical point (QCP), unconventional superconductivity, and emergent phenomena in vdW heterostructures. Here, we investigate 2D vdW heavy-fermion candidates through the database of experimentally known compounds based on dynamical mean-field theory calculation combined with density functional theory (DFT+DMFT). We have found that the Kondo resonance state of CeSiI does not change upon exfoliation and can be easily controlled by strain and surface doping. Our result indicates that CeSiI is an ideal 2D vdW heavy-fermion material and the quantum critical point can be identified by external perturbations.

Dirac cones can foster extraordinary electronic effects, as exemplified by the case of graphene layers. Angle-resolved photoemission reveals that adsorption of selenium (Se) vapor on bilayer graphene creates a symmetric hybrid clone of the Dirac cones at the zone center. A detailed analysis aided by first-principles calculations shows that the adsorbed layer consists of an ordered array of Se8 molecules. The uncovered cloning mechanism illustrates a method to generate electronic features of scientific and technological interests by gentle surface modification via van der Waals adsorption.

Current progress in two-dimensional (2D) materials explorations leads to constant specie enrichments of possible advanced materials down to two dimensions. The metal chalcogenide-based 2D materials are promising grounds where many adjacent territories are waiting to be explored. Here, a stable monolayer Ni3TeO6 (NTO) structure was computationally predicted and its stacked 2D nanosheets experimentally synthesized. Theoretical design undergoes featuring coordination of metalloid chalcogen, slicing the bulk structure, geometrical optimizations and stability study. The predicted layered NTO structure is realized in nanometer-thick nanosheets via a one-pot shape-controlled hydrothermal synthesis. Compared to the bulk, the 2D NTO own a lowered bandgap energy, more sensitive wavelength selectivity and an emerging photocatalytic hydrogen evolution ability under visible light. Beside a new 2D NTO with the optoelectrical and photocatalytic merits, its existing polar space group, structural specification, and design route are hoped to benefit 2D semiconductor innovations both in species enrichment and future applications.

The environment contributes to the screening of Coulomb interactions in two-dimensional semiconductors. This can potentially be exploited to tailor material properties as well as for sensing applications. Here, we investigate the tuning of the band gap and the exciton binding energy in the two-dimensional semiconductor WS2 via the external dielectric screening. Embedding WS2 in van der Waals heterostructures with graphene and hBN spacers of thicknesses between one and 16 atomic layers, we experimentally determine both energies as a function of the WS2-to-graphene interlayer distance and the charge carrier density in graphene. We find that the modification to the band gap as well as the exciton binding energy are well described by a one-over-distance dependence, with a significant effect remaining at several nanometers distance, at which the two layers are electrically well isolated. This observation is explained by a screening arising from an image charge induced by the graphene layer. Furthermore, we find that the effectiveness of graphene in screening Coulomb interactions in nearby WS2 depends on its doping level and can therefore be controlled via the electric field effect. We determine that, at room temperature, it is modified by approximately 20% for charge carrier densities of 2 × 1012 cm−2.

Focused ion beam (FIB) is an effective tool for precise nanoscale fabrication. It has recently been employed to tailor defect engineering in functional nanomaterials such as two-dimensional transition metal dichalcogenides (TMDCs), providing desirable properties in TMDC-based optoelectronic devices. However, the damage caused by the FIB irradiation and milling process to these delicate, atomically thin materials, especially in extended areas beyond the FIB target, has not yet been fully characterised. Understanding the correlation between lateral ion beam effects and optical properties of 2D TMDCs is crucial in designing and fabricating high-performance optoelectronic devices. In this work, we investigate lateral damage in large-area monolayer WS2 caused by the gallium focused ion beam milling process. Three distinct zones away from the milling location are identified and characterised via steady-state photoluminescence (PL) and Raman spectroscopy. The emission in these three zones have different wavelengths and decay lifetimes. An unexpected bright ring-shaped emission around the milled location has also been revealed by time-resolved PL spectroscopy with high spatial resolution. Our findings open up new avenues for tailoring the optical properties of TMDCs by charge and defect engineering via focused ion beam lithography. Furthermore, our study provides evidence that while some localised damage is inevitable, distant destruction can be eliminated by reducing the ion beam current. It paves the way for the use of FIB to create nanostructures in 2D TMDCs, as well as the design and realisation of optoelectrical devices on a wafer scale.

Single spin-defects in 2D transition-metal dichalcogenides are natural spin-photon interfaces for quantum applications. Here we report high-field magneto-photoluminescence spectroscopy from three emission lines (Q1, Q2, and Q*) of He-ion induced sulfur vacancies in monolayer MoS2. Analysis of the asymmetric PL lineshapes in combination with the diamagnetic shift of Q1 and Q2 yields a consistent picture of localized emitters with a wave function extent of ~3.5 nm. The distinct valley-Zeeman splitting in out-of-plane B-fields and the brightening of dark states through in-plane B-fields necessitates spin-valley selectivity of the defect states and lifted spin-degeneracy at zero field. Comparing our results to ab initio calculations identifies the nature of Q1 and Q2 and suggests that Q* is the emission from a chemically functionalized defect. Analysis of the optical degree of circular polarization reveals that the Fermi level is a parameter that enables the tunability of the emitter. These results show that defects in 2D semiconductors may be utilized for quantum technologies.