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α-RuCl3, a narrow-band Mott insulator with a large work function, offers intriguing potential as a quantum material or as a charge acceptor for electrical contacts in van der Waals devices. In this work, we perform a systematic study of the optical reflection contrast of α-RuCl3 nanoflakes on oxidized silicon wafers and estimate the accuracy of this imaging technique to assess the crystal thickness. Via spectroscopic micro-ellipsometry measurements, we characterize the wavelength-dependent complex refractive index of α-RuCl3 nanoflakes of varying thickness in the visible and near-infrared. Building on these results, we simulate the optical contrast of α-RuCl3 nanoflakes with thicknesses below 100 nm on SiO2/Si substrates under different illumination conditions. We compare the simulated optical contrast with experimental values extracted from optical microscopy images and obtain good agreement. Finally, we show that optical contrast imaging allows us to retrieve the thickness of the RuCl3 nanoflakes exfoliated on an oxidized silicon substrate with a mean deviation of −0.2 nm for thicknesses below 100 nm with a standard deviation of only 1 nm. Our results demonstrate that optical contrast can be used as a non-invasive, fast, and reliable technique to estimate the α-RuCl3 thickness. 

Abstract Advancements in low‐dimensional functional device technology heavily rely on the discovery of suitable materials which have interesting physical properties as well as can be exfoliated down to the 2D limit. Exfoliable high‐mobility magnets are one such class of materials that, not due to lack of effort, has been limited to only a handful of options. So far, most of the attention has been focused on the van der Waals (vdW) systems. However, even within the non‐vdW, layered materials, it is possible to find all these desirable features. Using chemical reasoning, it is found that NdSb₂is an ideal example. Even with a relatively small interlayer distance, this material can be exfoliated down to few layers. NdSb₂has an antiferromagnetic ground state with a quasi 2D spin arrangement. The bulk crystals show a very large, non‐saturating magnetoresistance along with highly anisotropic electronic transport properties. It is confirmed that this anisotropy originates from the 2D Fermi pockets which also imply a rather quasi 2D confinement of the charge carrier density. Both electron and hole‐type carriers show very high mobilities. The possible non‐collinear spin arrangement also results in an anomalous Hall effect. 

Abstract Magnetic van der Waals (vdW) materials are the centerpiece of atomically thin devices with spintronic and optoelectronic functions. Exploring new chemistry paths to tune their magnetic and optical properties enables significant progress in fabricating heterostructures and ultracompact devices by mechanical exfoliation. The key parameter to sustain ferromagnetism in 2D is magnetic anisotropy—a tendency of spins to align in a certain crystallographic direction known as easy‐axis. In layered materials, two limits of easy‐axis are in‐plane (XY) and out‐of‐plane (Ising). Light polarization and the helicity of topological states can couple to magnetic anisotropy with promising photoluminescence or spin‐orbitronic functions. Here, a unique experiment is designed to control the easy‐axis, the magnetic transition temperature, and the optical gap simultaneously in a series of CrCl_3−xBr_xcrystals between CrCl₃withXYand CrBr₃with Ising anisotropy. The easy‐axis is controlled between the two limits by varying spin–orbit coupling with the Br content in CrCl_3−xBr_x. The optical gap, magnetic transition temperature, and interlayer spacing are all tuned linearly withx. This is the first report of controlling exchange anisotropy in a layered crystal and the first unveiling of mixed halide chemistry as a powerful technique to produce functional materials for spintronic devices.