Over the past two decades, graphene has been intensively studied because of its remarkable mechanical, optical, and electronic properties. Initial studies were enabled by manual ``Scotch Tape'' exfoliation; nearly two decades later, this method is still widely used to obtain chemically-pristine flakes of graphene and other 2D van der Waals materials. Unfortunately, the yield of large, pristine flakes with uniform thickness is inconsistent. Thus, significant time and effort are required to exfoliate and locate flakes suitable for fabricating multilayer van der Waals heterostructures. Here, we describe a relatively affordable tabletop device (the ``eXfoliator'') that can reproducibly control key parameters and largely automate the exfoliation process. In a typical exfoliation run, the eXfoliator produces 3 or more large ($\ge400\ μ$m$^2$) high-quality graphene monolayer flakes, allowing new users to produce such flakes at a rate comparable to manual exfoliation by an experienced user. We use an automated mapping system and a computer vision algorithm to locate candidate flakes. Our results provide a starting point for future research efforts to more precisely identify which parameters matter for the success of exfoliation, and to optimize them.
Spin orbit interaction can be strongly boosted when a heavy element is embedded into an inversion asymmetric crystal field. A simple structure to realize this concept in a 2D crystal contains three atomic layers, a middle one built up from heavy elements generating strong atomic spin-orbit interaction and two neighboring atomic layers with different electron negativity. BiTeI is a promising candidate for such a 2D crystal, since it contains heavy Bi layer between Te and I layers. Recently the bulk form of BiTeI attracted considerable attention due to its giant Rashba interaction, however, 2D f…
We demonstrate a simple method to manipulate and exfoliate thick hexagonal boron nitride (h-BN) flakes using an atomic force microscope (AFM) cantilever and tip mounted to a micromanipulator stage. Thick flakes of tens to hundreds of nanometers can be thinned down to large area, few-layer and monolayer flakes. We characterize the resulting thinned-down flakes using AFM and Raman spectroscopy. This technique is extendable to other two dimensional, van der Waals materials.
We present a fabrication method producing large and flat graphene flakes that have a few layers down to a single layer based on substrate bonding of a thick sample of highly oriented pyrolytic graphite (HOPG), followed by its controlled exfoliation down to the few to single graphene atomic layers. As the graphite underlayer is intimately bonded to the substrate during the exfoliation process, the obtained graphene flakes are remarkably large and flat and present very few folds and pleats. The high occurrence of single layered graphene sheets having tens of micron wide in lateral dimensions is …
We evaluate the effect of mechanical exfoliation of van der Waals materials on crystallographic orientations of the resulting flakes. Flakes originating from a single crystal of graphite, whose orientation is confirmed using STM, are studied using facet orientations and electron back-scatter diffraction (EBSD). While facets exhibit a wide distribution of angles after a single round of exfoliation ($ σ\approx 5^o $), EBSD shows that the true crystallographic orientations are more narrowly distributed ($ σ\approx 1.5^o $), and facets have an approximately error from the true orientation. Further…
Graphite surfaces can be manipulated by several methods to create graphene structures of different shapes and sizes. Scanning tunneling microscopy (STM) can be used to create these structures either through mechanical contact between the tip and the surface or through electro-exfoliation. In the latter, the mechanisms involved in the process of exfoliation with an applied voltage are not fully understood. Here we show how a graphite surface can be locally exfoliated in a systematic manner by applying an electrostatic force with a STM tip at the edge of a terrace, forming triangular flakes seve…
Exfoliation of lamellar materials into their corresponding layers represented a breakthrough, due to the outstanding properties arising from the nanometric thickness confinement. Among the cleavage techniques, liquid-phase exfoliation is now on the rise because it is scalable and leads to easy-to-manipulate colloids. However, all appropriate exfoliating solvents exhibit strong polarity, which restrains a lot the scope of feasible functionalization or processing of the resulting flakes. Here we propose to extend this scope, demonstrating that nanosheets exfoliated in a polar medium can be prope…
Ferromagnetic van der Waals (vdW) materials are in demand for spintronic devices with all-two-dimensional-materials heterostructures. Here, we demonstrate mechanical exfoliation of magnetic-atom-intercalated transition metal dichalcogenide Cr1/3TaS2 from its bulk crystal; previously such intercalated materials were thought difficult to exfoliate. Magnetotransport in exfoliated tens-of-nanometres-thick flakes revealed ferromagnetic ordering below its Curie temperature TC ~ 110 K as well as strong in-plane magnetic anisotropy; these are identical to its bulk properties. Further, van der Waals he…
We investigate the micromechanical exfoliation and van der Waals (vdW) assembly of ferromagnetic layered dichalcogenide Fe0.25TaS2. The vdW interlayer coupling at the Fe-intercalated plane of Fe0.25TaS2 allows exfoliation of flakes. A vdW junction between the cleaved crystal surfaces is constructed by dry transfer method. We observe tunnel magnetoresistance in the resulting junction under an external magnetic field applied perpendicular to the plane, demonstrating spin-polarized tunneling between the ferromagnetic layered material through the vdW junction.
We investigated multilayer plates made by exfoliation from a high-quality MoS$_2$ crystal and reveal that they represent a new object - van der Waals homostructure consisting of a bulk core and a few detached monolayers on its surface. This architecture comprising elements with different electron band structure leads to specific luminescence, when the broad emission band from the core is cut by the absorption peaks of strong exciton resonances in the surface monolayers. The exfoliated flakes exhibit strong optical anisotropy. We have observed a conversion of normally incident light polarizatio…
We report the isolation of thin flakes of cylindrite, a naturally occurring van der Waals superlattice, by means of mechanical and liquid phase exfoliation. We find that this material is a heavily doped p-type semiconductor with a narrow gap (<0.85 eV) with intrinsic magnetic interactions that are preserved even in the exfoliated nanosheets. Due to its environmental stability and high electrical conductivity, cylindrite can be an interesting alternative to the existing two-dimensional magnetic materials.
We show that it is possible to deposit, by mechanical exfoliation on SiO2/Si wafers, atomically thin mica flakes down to a single monolayer thickness. The optical contrast of these mica flakes on top of a SiO2/Si substrate, which depends on their thickness, the illumination wavelength and the SiO2 substrate thickness, can be quantitatively accounted for by a Fresnel law based model. The preparation of atomically thin insulating crystalline sheets will enable the fabrication of ultrathin defect-free insulating substrates, dielectric barriers or planar electron tunneling junctions. Additionally,…
Folded graphene flakes are a natural byproduct of the micromechanical exfoliation process. In this Letter we show by a combination of analytical and numerical methods that such systems behave as intriguing interferometers due to the interplay between an externally applied magnetic field and the gauge field induced by the deformations in the region of the fold.
Deposition of clean and defect-free atomically thin two-dimensional crystalline flakes on surfaces by mechanical exfoliation of layered bulk materials has proven to be a powerful technique, but it requires a fast, reliable and non-destructive way to identify the atomically thin flakes among a crowd of thick flakes. In this work, we provide general guidelines to identify ultrathin flakes of TaSe2 by means of optical microscopy and Raman spectroscopy. Additionally, we determine the optimal substrates to facilitate the optical identification of atomically thin TaSe2 crystals. Experimental realiza…
Phosphorene, a two-dimensional (2D) monolayer of black phosphorus, has attracted considerable theoretical interest, although the experimental realization of monolayer, bilayer, and few-layer flakes has been a significant challenge. Here we systematically survey conditions for liquid exfoliation to achieve the first large-scale production of monolayer, bilayer, and few-layer phosphorus, with exfoliation demonstrated at the 10-gram scale. We describe a rapid approach for quantifying the thickness of 2D phosphorus and show that monolayer and few-layer flakes produced by our approach are crystalli…
Two-dimensional (2D) magnetic van der Waals materials provide a powerful platform for studying fundamental physics of low-dimensional magnetism, engineering novel magnetic phases, and enabling ultrathin and highly tunable spintronic devices. To realize high quality and practical devices for such applications, there is a critical need for robust 2D magnets with ordering temperatures above room temperature that can be created via exfoliation. Here the study of exfoliated flakes of cobalt substituted Fe5GeTe2 (CFGT) exhibiting magnetism above room temperature is reported. Via quantum magnetic ima…
There is an increasing interest to develop nanoscale biocompatible graphene structures due to their desirable physicochemical properties, unlimited application opportunities and scalable production. Here we report the preparation, characterization and biocompatibility assessment of novel graphene flakes and their enabled thin films suitable for a wide range of biomedical and electronic applications. Graphene flakes were synthesized by a chemical vapour deposition method or a liquid-phase exfoliation procedure and then thin films were prepared by transferring graphene onto glass coverslips. Ram…
A fluid-based method is demonstrated for preparing graphene nanomeshes (GNMs) directly from pristine graphite flakes by a one-step process. The high efficiency is attributed to the combination of fluid-assisted exfoliation and perforation of the graphene sheets. Atomic force microscopy shows that the as-produced GNMs are less than 1.5 nm thick. The total area of the pores within 1 um2 of the GNM sheet is estimated as ~0.15 um2 and the pore density as ~22 um-2, The yield of GNMs from pristine graphite powder and the power consumption for per gram GNM synthesis are evaluated as 5 wt% and 120 kWh…
Vertically stacked van der Waals heterostructures are a lucrative platform for exploring the rich electronic and optoelectronic phenomena in two-dimensional materials. Their performance will be strongly affected by impurities and defects at the interfaces. Here we present the first systematic study of interfaces in van der Waals heterostructure using cross sectional scanning transmission electron microscope (STEM) imaging. By measuring interlayer separations and comparing these to density functional theory (DFT) calculations we find that pristine interfaces exist between hBN and MoS2 or WS2 fo…
The dry release transfer of two-dimensional (2D) materials such as graphene, h-BN, and TMDs is a versatile method for fabricating high-quality van der Waals heterostructures. Up until now, polydimethylpolysiloxane (PDMS) sheets have been widely used for the dry release transfer of TMD materials. However, this method has been known to have limitations that make it difficult to transfer few-layer-thick graphene and h-BN because of the difficulty to fabricate these materials on PDMS. As an alternative method, we demonstrate the dry release transfer of single- and bi-layer graphene and few-layer h…
