Zemin Pan#, Wenqi Xiong#, Jiaqi Dai#, Hui Zhang#, Yunhua Wang, Tao Jian, Xingxia Cui, Jinghao Deng, Xiaoyu Lin, Zhengbo Cheng, Yusong Bai, Chao Zhu, Da Huo, Geng Li, Min Feng, Jun He, Wei Ji*, Shengjun Yuan*, Fengcheng Wu*, Chendong Zhang*, and Hong-Jun Gao
Abstract:
Although the kagome model is fundamentally two-dimensional, the essential kagome physics, i.e., the kagome-bands-driven emergent electronic states, has yet to be explored in the monolayer limit. Here, we present the experimental realization of kagome physics in monolayer Mo33Te56, showcasing both ferromagnetic ordering and a correlated insulating state with an energy gap of up to 15 meV. Using a combination of scanning tunnelling microscopy and theoretical calculations, we find a structural phase of the monolayer Mo-Te compound, which forms a mirror-twin boundary loop superlattice exhibiting kagome geometry and multiple sets of kagome bands. The partial occupancy of these nearly flat bands results in Fermi surface instability, counteracted by the emergence of ferromagnetic order (with a coercive field ~0.1 T, as observed by spin-polarized STM) and the opening of a correlated hard gap. Our work establishes a robust framework featuring well-defined atomic and band structures, alongside the intrinsic two-dimensional nature, essential for the rigorous examination of kagome physics.
Renhong Wang (王人宏), Cong Wang (王聪)*, Ruixuan Li (李睿宣), Deping Guo (郭的坪), Jiaqi Dai (戴佳琦), Canbo Zong (宗灿波), Weihan Zhang (张伟 涵), and Wei Ji (季威)*
Abstract:
Kagome materials are known for hosting exotic quantum states, including quantum spin liquids, charge density waves, and unconventional superconductivity. The search for kagome monolayers is driven by their ability to exhibit neat and well-defined kagome bands near the Fermi level, which are more easily realized in the absence of interlayer interactions. However, this absence also destabilizes the monolayer forms of many bulk kagome materials, posing significant challenges to their discovery. In this work, we propose a strategy to address this challenge by utilizing oxygen vacancies in transition metal oxides within a “1+3” design framework. Through high-throughput computational screening of 349 candidate materials, we identified 12 thermodynamically stable kagome monolayers with diverse electronic and magnetic properties. These materials were classified into three categories based on their lattice geometry, symmetry, band gaps, and magnetic configurations. Detailed analysis of three representative monolayers revealed kagome band features near their Fermi levels, with orbital contributions varying between oxygen 2p and transition metal d states. This study demonstrates the feasibility of the “1+3” strategy, offering a promising approach to uncovering low-dimensional kagome materials and advancing the exploration of their quantum phenomena.
Individual superatoms were assembled into more complicated nanostructures for diversify their physical properties. Magnetism of assembled superatoms remains, however, ambiguous, particularly in terms of its distance dependence. Here, we report density functional theory calculations on the distance-dependent magnetism of transition metal embedded Au6Te8Se12 (ATS) superatomic dimers. Among the four considered transition metals, which include V, Cr, Mn and Fe, the Cr-embedded Au6Te12Se8 (Cr@ATS) is identified as the most suitable for exploring the inter-superatomic distance-dependent magnetism. We thus focused on Cr@ATS superatomic dimers and found an inter-superatomic magnetization-distance oscillation where three transitions occur for magnetic ordering and/or anisotropy at different inter-superatomic distances. As the inter-superatomic distance elongates, a ferromagnetism (FM)-to-antiferromagnetic (AFM) transition and a sequential AFM-to-FM transition occur, ascribed to competitions among Pauli repulsion and kinetic-energy-gains in formed inter-superatomic Cr-Au-Au-Cr covalent bonds and Te-Te quasi-covalent bonds. For the third transition, in-plane electronic hybridization contributes to the stabilization of the AFM configuration. This work unveils two mechanisms for tuning magnetism through non-covalent interactions and provides a strategy for manipulating magnetism in superatomic assemblies.
Yueshen Wu, Yuxiong Hu, Cong Wang, Xiang Zhou, Xiaofei Hou, Wei Xia, Yiwen Zhang, Jinghui Wang, Yifan Ding, Jiadian He, Peng Dong, Song Bao, Jinsheng Wen, Yanfeng Guo, Kenji Watanabe, Takashi Taniguchi, Wei Ji, Zhu-Jun Wang, Jun Li
Abstract:
Fe3GeTe2 have proven to be of greatly intrigue. However, the underlying mechanism behind the varying Curie temperature (Tc) values remains a puzzle. Here, we explored the atomic structure of Fe3GeTe2 crystals exhibiting Tc values of 160, 210, and 230 K. The elemental mapping reveals a Fe-intercalation on the interstitial sites within the van der Waals gap of the high- Tc (210 and 230 K) samples, which are observed an exchange bias effect by electrical transport measurements, while Fe intercalation or the bias effect is absent in the low-Tc (160 K) samples. First-principles calculations further suggest that the Fe-intercalation layer may be responsible for the local antiferromagnetic coupling that gives rise to the exchange bias effect, and that the interlayer exchange paths greatly contributes to the enhancement of Tc. This discovery of the Fe-intercalation layer elucidates the mechanism behind the hidden antiferromagnetic ordering that underlies the enhancement of Tc in Fe3GeTe2.
The fabrication of one-dimensional (1D) magnetic systems on solid surfaces, although of high fundamental interest, has yet to be achieved for a crossover between two-dimensional (2D) magnetic layers and their associated 1D spin chain systems. In this study, we report the fabrication of 1D single-unit-cellwidth CrCl3 atomic wires and their stacked few-wire arrays on the surface of a van der Waals (vdW) superconductor NbSe2. Scanning tunneling microscopy/spectroscopy and first-principles calculations jointly revealed that the single wire shows an antiferromagnetic large-bandgap semiconducting state in an unexplored structure different from the well-known 2D CrCl3 phase. Competition among the total energies and nanostructure-substrate interfacial interactions of these two phases result in the appearance of the 1D phase. This phase was transformable to the 2D phase either prior to or after the growth for in situ or ex situ manipulations, in which the electronic interactions at the vdW interface play a nontrivial role that could regulate the dimensionality conversion and structural transformation between the 1D-2D CrCl3 phases.
