The research about two-dimensional van der Waals magnetic materials has advanced the 22 breakthroughs in ultrathin magnetic devices. We experimentally demonstrate that single-crystal 23 N-face AlN polar substrate can program layer-number-parity-dependent magnetic multistates and 24 their evolution sequence in few-layer CrI3. In odd-layer samples, as 5L-CrI3/AlN, when μ0H 25 sweeps from 3 to −3 T, the reflective magnetic circular dichroism signal evolves through distinct 26 magnetic multistates (+5 → –1 → +1 → –5), where +1 corresponds to the moment of a spin-up 27 monolayer. Thereby, we vertically program novel magnetic ground states and their evolution 28 sequence via a simplified heterointerface. Our first-principles calculations attribute this effect to 29 interfacial hole doping: it globally reconfigures the magnetic ground state of odd-layer CrI3 to a 30 novel ferrimagnetic order, and spatially differentiates the interlayer exchange and magnetic 31 anisotropy between the surface/interfacial and interior layers. Our work advances the practical 32 integration and design of two-dimensional magnetic devices with tailored functionalities.
The chromium-based kagome metal CsCr3Sb5 has garnered significant interest due to its strong electron correlations, intertwined orders and potential for unconventional superconductivity under high pressure. The evolution of magnetic and superconducting interactions as the more frequently studied CsCr3Sb5 is doped to CsCr3Sb5 remains poorly understood. Here, we demonstrate the emergence of a spatially anisotropic Kondo resonance intertwined with the superconducting gap, enabled by introducing magnetic Cr impurities into the kagome superconductor CsCr3Sb5. The addition of dilute Cr impurities not only weakens long range charge density wave order but also produces local magnetic moments that leads to Kondo resonances. We show that the Kondo resonance forms anisotropic, ripple like spatial patterns around individual Cr atoms, breaking all local mirror symmetries. We further reveal that with the emergence of Kondo screening, the coherence peak and depth of superconducting gap with finite zero-energy conductance are enhanced. This suggests that non superconducting carriers at the Fermi surface in the parent compound participate in the Kondo effect, simultaneously screening Cr magnetic moments and increasing the superfluid density. Our findings offer an opportunity to study the interplay between superconductivity and local magnetism in kagome materials.
Kagome lattices facilitate various quantum phases, yet in bulk materials, their kagome flat-bands often interact with bulk bands, suppressing kagome electronic characteristics for hosting these phases. Here, we use density-functional-theory calculations to predict the geometric and electronic structures, as well as the topological and magnetic properties, of a series of MoTe2-x kagome monolayers formed by mirror-twin-boundary (MTB) loops. We analyze nine MTB-loop configurations of varying sizes and arrangements to assess their impact on various properties. Within the intrinsic bandgap of MoTe2, we identify two sets of kagome bands, originating from in-plane and out-of-plane Te p-orbitals at MTB-loop edges and -vertices, respectively. Three configurations exhibit superior stability, while three others show comparable stability. Among these, four display bandgaps and potentially non-zero Z2 topological invariants, suggesting possible topological phases, while the remaining two are metallic and feature Stoner magnetization. These findings guide the design of kagome-based two-dimensional materials with tunable electronic, topological, and magnetic properties.
Breathing kagome materials Nb3X8 (X = F, Cl, Br, I) have attracted broad interest owing to their Mott insulating behavior and stacking-dependent magnetic ground states. However, the role of interlayer coupling in modulating these properties remains underexplored. Here, using density functional theory with Hubbard U corrections, we systematically investigated how interlayer coupling affects the Mott insulating states and magnetic ground states across 24 bilayer stacking configurations for each compound. We found that all bilayers remain Mott insulators, demonstrating robust Mottness. Driven by the competition between interlayer Pauli repulsion and hopping, most stackings favor interlayer AFM order, including conventional and compensated AFM, while some exhibit AFM-FM degeneracy or stabilize interlayer FM. This robustness of Mott states coexisting with tunable interlayer magnetism provides novel analysis and insights for research on breathing kagome Mott insulators.
Deju Zhang, Zhe Wang, Sihang Che, Wei Ji, and Yanning Zhang*
Abstract:
In the field of low-energy-consumption applications, electrical control of magnetism has attracted considerable research attention. Here, we report that the Janus Cr2S2Se monolayer, where Se atoms substitute the upper S layer in the Cr2S3 monolayer, is structural stable. We find that the Janus Cr2S2Se monolayer favors the ferromagnetic configuration with a high Curie temperature of 279 K, and shows semiconducting characteristics with an indirect band gap of 0.44 eV and a valley splitting of 33 meV. By constructing a van der Waals multiferroic heterostructure combined with α-In2Se3 monolayer, its interlayer magnetism can be switched between two types of magnetic coupling via nonvolatile manipulation of the ferroelectric polarization. Our study reveals the switchable magnetism of the Janus Cr2S2Se monolayer, making it promising candidates for use in next-generation low-dimensional spintronics applications.
