High-Entropy van der Waals Materials Formed from Mixed Metal Dichalcogenides, Halides, and Phosphorus Trisulfides.

The charge, spin, and composition degrees of freedom in a 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 a van der Waals material bring to it exceptional features and technological applications. Integration of these two distinct material categories while keeping their merits would be tempting. On the basis of 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 a homogeneous element distribution can be efficiently acquired and easily exfoliated or intercalated in this materials category. Multifarious physical properties such as 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.