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Nanoporous membranes based on two dimensional materials are predicted to provide highly selective gas transport in combination with extreme permeability. Here we investigate membranes made from multilayer graphdiyne, a graphene-like crystal with a larger unit cell. Despite being nearly a hundred of nanometers thick, the membranes allow fast, Knudsen-type permeation of light gases such as helium and hydrogen whereas heavy noble gases like xenon exhibit strongly suppressed flows. Using isotope and cryogenic temperature measurements, the seemingly conflicting characteristics are explained by a high density of straight-through holes (direct porosity of ~0.1%), in which heavy atoms are adsorbed on the walls, partially blocking Knudsen flows. Our work offers important insights into intricate transport mechanisms playing a role at nanoscale.

Suspended specimens of 2D crystals and their heterostructures are required for a range of studies including transmission electron microscopy (TEM), optical transmission experiments and nanomechanical testing. However, investigating the properties of laterally small 2D crystal specimens, including twisted bilayers and air sensitive materials, has been held back by the difficulty of fabricating the necessary clean suspended samples. Here we present a scalable solution which allows clean free-standing specimens to be realized with 100% yield by dry-stamping atomically thin 2D stacks onto a specially developed adhesion-enhanced support grid. Using this new capability, we demonstrate atomic resolution imaging of defect structures in atomically thin CrBr3, a novel magnetic material which degrades in ambient conditions., Comment: 17 pages (+ references), 3 Figures, 1 Table

The convergent beam electron diffraction (CBED) patterns of twisted bilayer samples exhibit interference patterns in their CBED spots. Such interference patterns can be treated as off-axis holograms and the phase of the scattered waves, meaning the interlayer distance can be reconstructed. A detailed protocol of the reconstruction procedure is provided in this study. In addition, we derive an exact formula for reconstructing the interlayer distance from the recovered phase distribution, which takes into account the different chemical compositions of the individual monolayers. It is shown that one interference fringe in a CBED spot is sufficient to reconstruct the distance between the layers, which can be practical for imaging samples with a relatively small twist angle or when probing small sample regions. The quality of the reconstructed interlayer distance is studied as a function of the twist angle. At smaller twist angles, the reconstructed interlayer distance distribution is more precise and artefact free. At larger twist angles, artefacts due to the moir\'e structure appear in the reconstruction. A method for the reconstruction of the average interlayer distance is presented. As for resolution, the interlayer distance can be reconstructed by the holographic approach at an accuracy of 0.5 A, which is a few hundred times better than the intrinsic z-resolution of diffraction limited resolution, as expressed through the spread of the measured k-values. Moreover, we show that holographic CBED imaging can detect variations as small as 0.1 A in the interlayer distance, though the quantitative reconstruction of such variations suffers from large errors.

In this work, the room temperature polar vapor sensing behavior of two dimentional (2D) heterojunction Graphene-TiS3 materials and TiS3 nanoribbons is investigated. TiS3 nanoribbons were synthesized via chemical vapor transport (CVT) and their structure was investigated by scanning electron microscopy (SEM), high resolution transmission electron microscopy (HRTEM), energy dispersive X- ray spectroscopy (EDS), X-ray diffraction (XRD), Raman spectroscopy and Fourier transform infrared spectroscopy (FT-IR) analysis. The gas sensing performance of the TiS3 nanoribbons was assessed through the observed changes in their electronic behavior. Sensing devices were fabricated with gold contacts and with lithographically patterned graphene (Gr) electrodes in a 2D heterojunction Gr-TiS3-Gr architecture.. It is observed that the gold contacted TiS3 device has a rather linear I-V behavior while the Gr-TiS3-Gr heterojunction forms a contact with a higher Schottky barrier (250 meV). I-V responses of the sensors were recorded at room temperature with a relative humidity of 55% and for different ethanol vapor concentrations (varying from 2 to 20 ppm). I-V plots indicated an increase in the resistance of Gr-TiS3-Gr by the adsorption of water and ethanol molecules with relatively high sensing response (~3353% at 2 ppm). Our results reveal that selective and stable responses to a low concentration of ethanol vapor (2 ppm) can be achieved at room temperature with transient response and recovery times of around 6 s and 40 s, respectively. Our proposed design demonstrate a new approach for selective molecular recognition using polar interactions between analyte vapors and heterojunctions of 2D-materials.

Van der Waals heterostructures form a massive interdisciplinary research field, fueled by the rich material science opportunities presented by layer assembly of artificial solids with controlled composition, order and relative rotation of adjacent atomic planes. Here we use atomic resolution transmission electron microscopy and multiscale modeling to show that the lattice of MoS$_2$ and WS$_2$ bilayers twisted to a small angle, $\theta<3^{\circ}$, reconstructs into energetically favorable stacking domains separated by a network of stacking faults. For crystal alignments close to 3R stacking, a tessellated pattern of mirror reflected triangular 3R domains emerges, separated by a network of partial dislocations which persist to the smallest twist angles. Scanning tunneling measurements show that the electronic properties of those 3R domains appear qualitatively different from 2H TMDs, featuring layer-polarized conduction band states caused by lack of both inversion and mirror symmetry. In contrast, for alignments close to 2H stacking, stable 2H domains dominate, with nuclei of an earlier unnoticed metastable phase limited to $\sim$ 5nm in size. This appears as a kagome-like pattern at $\theta\sim 1^{\circ}$, transitioning at $\theta\rightarrow 0$ to a hexagonal array of screw dislocations separating large-area 2H domains.

Control over the electronic spectrum at low energy is at the heart of the functioning of modern advanced electronics: high electron mobility transistors, semiconductor and Capasso terahertz lasers, and many others. Most of those devices rely on the meticulous engineering of the size quantization of electrons in quantum wells. This avenue, however, hasn't been explored in the case of 2D materials. Here we transfer this concept onto the van der Waals heterostructures which utilize few-layers films of InSe as quantum wells. The precise control over the energy of the subbands and their uniformity guarantees extremely high quality of the electronic transport in such systems. Using novel tunnelling and light emitting devices, for the first time we reveal the full subbands structure by studying resonance features in the tunnelling current, photoabsorption and light emission. In the future, these systems will allow development of elementary blocks for atomically thin infrared and THz light sources based on intersubband optical transitions in few-layer films of van der Waals materials., Comment: 12 pages, 3 figures

Vertically stacking two dimensional (2D) materials can enable the design of novel electronic and optoelectronic devices and realize complex functionality. However, the fabrication of such artificial heterostructures in wafer scale with an atomically-sharp interface poses an unprecedented challenge. Here, we demonstrate a convenient and controllable approach for the production of wafer-scale 2D GaSe thin films by molecular beam epitaxy. In-situ reflection high-energy electron diffraction oscillations and Raman spectroscopy reveal a layer-by-layer van der Waals epitaxial growth mode. Highly-efficient photodetector arrays were fabricated based on few-layer GaSe on Si. These photodiodes show steady rectifying characteristics and a relatively high external quantum efficiency of 23.6%. The resultant photoresponse is super-fast and robust with a response time of 60 us. Importantly, the device shows no sign of degradation after 1 million cycles of operation. Our study establishes a new approach to produce controllable, robust and large-area 2D heterostructures and presents a crucial step for further practical applications.

Three dimensional (3D) Dirac semimetals are 3D analogue of graphene, which display Dirac points with linear dispersion in k-space, stabilized by crystal symmetry. Cd3As2 and Na3Bi were predicted to be 3D Dirac semimetals and were subsequently demonstrated by photoemission experiments. As unveiled by transport measurements, several exotic phases, such as Weyl semimetals, topological insulators, and topological superconductors, can be deduced by breaking time reversal or inversion symmetry. Here, we reported a facile and scalable chemical vapor deposition method to fabricate high-quality Dirac semimetal Cd3As2 microbelts, they have shown ultrahigh mobility up to 1.15*10^5 cm^2/V s and pronounced Shubnikov-de Haas oscillations. Such extraordinary features are attributed to the suppression of electron backscattering. This research opens a new avenue for the scalable fabrication of Cd3As2 materials towards exciting electronic applications of 3D Dirac semimetals., Comment: 15 pages, 4 Figures

Two-dimensional (2D) materials have attracted substantial attention in electronic and optoelectronic applications with superior advantages of being flexible, transparent and highly tunable. Gapless graphene exhibits ultra-broadband and fast photoresponse while the 2D semiconducting MoS2 and GaTe unveil high sensitivity and tunable responsivity to visible light. However, the device yield and the repeatability call for a further improvement of the 2D materials to render large-scale uniformity. Here we report a layer-by-layer growth of wafer-scale GaTe with a hole mobility of 28.4 cm2/Vs by molecular beam epitaxy. The arrayed p-n junctions were developed by growing few-layer GaTe directly on three-inch Si wafers. The resultant diodes reveal good rectifying characteristics, photoresponse with a maximum photoresponsivity of 2.74 A/W and a high photovoltaic external quantum efficiency up to 62%. The photocurrent reaches saturation fast enough to capture a time constant of 22 {\mu}s and shows no sign of device degradation after 1.37 million cycles of operation. Most strikingly, such high performance has been achieved across the entire wafer, making the volume production of devices accessible. Finally, several photo-images were acquired by the GaTe/Si photodiodes with a reasonable contrast and spatial resolution, demonstrating for the first time the potential of integrating the 2D materials with the silicon technology for novel optoelectronic devices.