No Arabic abstract
Understanding the electronic transport properties of layered, van der Waals transition metal halides (TMHs) and chalcogenides is a highly active research topic today. Of particular interest is the evolution of those properties with changing thickness as the 2D limit is approached. Here, we present the electrical conductivity of exfoliated single crystals of the TMH, cluster magnet, Nb3Cl8, over a wide range of thicknesses both with and without hexagonal boron nitride (hBN) encapsulation. The conductivity is found to increase by more than three orders of magnitude when the thickness is decreased from 280 {mu}m to 5 nm, at 300 K. At low temperatures and below ~50 nm, the conductance becomes thickness independent, implying surface conduction is dominating. Temperature dependent conductivity measurements indicate Nb3Cl8 is an insulator, however the effective activation energy decreases from a bulk value of 310 meV to 140 meV by 5nm. X-ray photoelectron spectroscopy (XPS) shows mild surface oxidation in devices without hBN capping, however, no significant difference in transport is observed when compared to the capped devices, implying the thickness dependent transport behavior is intrinsic to the material. A conduction mechanism comprised of a higher conductivity surface channel in parallel with a lower conductivity interlayer channel is discussed.
The crystallographic and magnetic properties of the cleavable 4d3 transition metal compound a-MoCl3 are reported, with a focus on the behavior above room temperature. Crystals were grown by chemical vapor transport and characterized using temperature dependent x-ray diffraction, Raman spectroscopy, and magnetization measurements. A structural phase transition occurs near 585 K, at which the Mo-Mo dimers present at room temperature are broken. A nearly regular honeycomb net of Mo is observed above the transition, and an optical phonon associated with the dimerization instability is identified in the Raman data and in first-principles calculations. The crystals are diamagnetic at room temperature in the dimerized state, and the magnetic susceptibility increases sharply at the structural transition. Moderately strong paramagnetism in the high-temperature structure indicates the presence of local moments on Mo. This is consistent with results of spin-polarized density functional theory calculations using the low- and high-temperature structures. Above the magnetostructural phase transition the magnetic susceptibility continues to increase gradually up to the maximum measurement temperature of 780 K, with a temperature dependence that suggests two-dimensional antiferromagnetic correlations.
Magnetic van der Waals (vdW) materials have been heavily pursued for fundamental physics as well as for device design. Despite the rapid advances, so far magnetic vdW materials are mainly insulating or semiconducting, and none of them possesses a high electronic mobility - a property that is rare in layered vdW materials in general. The realization of a magnetic high-mobility vdW material would open the possibility for novel magnetic twistronic or spintronic devices. Here we report very high carrier mobility in the layered vdW antiferromagnet GdTe3. The electron mobility is beyond 60,000 cm2 V-1 s-1, which is the highest among all known layered magnetic materials, to the best of our knowledge. Among all known vdW materials, the mobility of bulk GdTe3 is comparable to that of black phosphorus, and is only surpassed by graphite. By mechanical exfoliation, we further demonstrate that GdTe3 can be exfoliated to ultrathin flakes of three monolayers, and that the magnetic order and relatively high mobility is retained in approximately 20-nm-thin flakes.
Van der Waals (vdW) layered materials have rather weaker interlayer bonding than the intra-layer bonding, therefore the exfoliation along the stacking direction enables the achievement of monolayer or few layers vdW materials with emerging novel physical properties and functionalities. The ferroelectricity in vdW materials recently attracts renewed interest for the potential use in high-density storage devices. As the thickness going thinner, the competition between the surface energy, depolarization field and interfacial chemical bonds may give rise to the modification of ferroelectricity and crystalline structure, which has limited investigations. In this work, combining the piezoresponse force microscope scanning, contact resonance imaging, we report the existence of the intrinsic in-plane polarization in vdW ferroelectrics CuInP2S6 (CIPS) single crystals, whereas below a critical thickness between 90-100 nm, the in-plane polarization disappears. The Youngs modulus also shows an abrupt stiffness at the critical thickness. Based on the density functional theory calculations, we ascribe these behaviors to a structural phase transition from monoclinic to trigonal structure, which is further verified by transmission electron microscope technique. Taken together, these findings demonstrate the foundational importance of structural phase transition for enhancing the rich functionality and broad utility of vdW ferroelectrics.
Two-dimensional (2D) MoSi$_2$N$_4$ monolayer is an emerging class of air-stable 2D semiconductor possessing exceptional electrical and mechanical properties. Despite intensive recent research efforts devoted to uncover the material properties of MoSi$_2$N$_4$, the physics of electrical contacts to MoSi$_2$N$_4$ remains largely unexplored thus far. In this work, we study the van der Waals heterostructures composed of MoSi$_2$N$_4$ contacted by graphene and NbS$_2$ monolayers using first-principle density functional theory calculations. We show that the MoSi$_2$N$_4$/NbS$_2$ contact exhibits an ultralow Schottky barrier height (SBH), which is beneficial for nanoelectronics applications. For MoSi$_2$N$_4$/graphene contact, the SBH can be modulated via interlayer distance or via external electric fields, thus opening up an opportunity for reconfigurable and tunable nanoelectronic devices. Our findings provide insights on the physics of 2D electrical contact to MoSi$_2$N$_4$, and shall offer a critical first step towards the design of high-performance electrical contacts to MoSi$_2$N$_4$-based 2D nanodevices.
The exfoliation of two naturally occurring van der Waals minerals, graphite and molybdenite, arouse an unprecedented level of interest by the scientific community and shaped a whole new field of research: 2D materials research. Several years later, the family of van der Waals materials that can be exfoliated to isolate 2D materials keeps growing, but most of them are synthetic. Interestingly, in nature plenty of naturally occurring van der Waals minerals can be found with a wide range of chemical compositions and crystal structures whose properties are mostly unexplored so far. This Perspective aims to provide an overview of different families of van der Waals minerals to stimulate their exploration in the 2D limit.