Abstract
Interlayer interactions in two-dimensional (2D) materials have long been oversimplified as weak van der Waals forces, leading to a significant underestimation of their role in shaping electronic structure, magnetism, and electric polarization. Building upon our understanding of non-covalent interactions across vdW gaps and heterointerfaces, we have proposed novel interlayer magnetic exchange mechanisms and uncovered unconventional modulation phenomena in low-dimensional systems. Our work identified interlayer stacking, layer number, and interlayer distance as sensitive degrees of freedom for tailoring magnetism in 2D magnets. These mechanisms were theoretically established and experimentally validated in CrI3, CrSe2, and CrTe2. The easy magnetization axis in MnSe2 was shown to be dictated by interfacial Se p-orbital hybridization. Heterointerfaces further extend the tuning dimension: we established strain-mediated phase diagrams for intra- and interlayer magnetism in CrSe2 and CrTe2. We demonstrated that epitaxial strain, interfacial charge transfer, and intercalation can effectively modulate the magnetic ground state and Curie temperature of Fe3GeTe2 and CrI3. Beyond magnetism, we have shown that interlayer non-covalent interactions can markedly alter the switching barrier between ferroelectric and antiferroelectric phases in Bi2TeO5. Extending the non-covalent tuning concept to zero-dimensional host–guest systems, we realized the first single-molecule electret in Gd@C82 and achieved probabilistic-state-based computation in Sc2C2@C88
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