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High-entropy van der Waals materials formed from mixed metal dichalcogenides, halides and phosphorus trisulfides

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 Added by Tianping Ying
 Publication date 2021
  fields Physics
and research's language is English




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The charge, spin, and composition degrees of freedom in high-entropy alloy endow it with tunable valence and spin states, infinite combinations and excellent mechanical performance. Meanwhile, the stacking, interlayer, and angle degrees of freedom in van der Waals material bring it with exceptional features and technological applications. Integration of these two distinct material categories while keeping their merits would be tempting. Based on this heuristic thinking, we design and explore a new range of materials (i.e., dichalcogenides, halides and phosphorus trisulfides) with multiple metallic constitutions and intrinsic layered structure, which are coined as high-entropy van der Waals materials. Millimeter-scale single crystals with homogeneous element distribution can be efficiently acquired and easily exfoliated or intercalated in this materials category. Multifarious physical properties like superconductivity, magnetic ordering, metal-insulator transition and corrosion resistance have been exploited. Further research based on the concept of high-entropy van der Waals materials will enrich the high-throughput design of new systems with intriguing properties and practical applications.



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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.
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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.
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