Interlayer coupling plays a critical role in tuning the electronic structures and magnetic ground states of two-dimensional materials, influenced by the number of layers, interlayer distance, and stacking order. However, its effect on the orientation of the magnetic easy axis remains underexplored. In this study, we demonstrate that interlayer coupling can significantly alter the magnetic easy-axis orientation, as shown by the magnetic easy-axis of monolayer 1T-MnSe2 tilting 33° from the z-axis, while aligning with the z-axis in the bilayer. This change results from variations in orbital occupations near the Fermi level, particularly involving nonmetallic Se atoms. Contrary to the traditional focus on magnetic metal atoms, our findings reveal that Se orbitals play a key role in influencing the easy-axis orientation and topological Chern numbers. Furthermore, we show that the occupation of Se p-orbitals, and consequently the magnetic anisotropy, can be modulated by factors such as stacking order, charge doping, and external strain. Our results highlight the pivotal role of interlayer coupling in tuning the magnetic properties of layered materials, with important implications for spintronic applications.
Altermagnetism has recently attracted significant interest in three- and two-dimensional materials, yet its realization in quasi-one-dimensional (Q1D) materials remains largely unexplored due to stringent symmetry constraints. Here, we systematically investigated the emergence of altermagnetism in 30 Q1D monolayer prototypes, self-assembled from intra-chain anti-ferrimagnetically coupled XYn single-atomic magnetic chains, using symmetry analysis and high-throughput density functional theory calculations. Symmetry analysis identifies four structural prototypes capable of hosting altermagnetism, which expand to 192 monolayers upon materialization. Our calculations further reveal eight dynamically stable Q1D altermagnets, all belonging the AA-stacked intra-chain AFM coupled β-XY₃ prototype, exhibiting d-wave-like spin splitting. Furthermore, we demonstrate the tunability of altermagnetic properties by varying inter-chain spacing and applying external electric fields. By optimizing these parameters, altermagnetism can be significantly enhanced, with spin splitting reaching several hundred meV in CoTe3, or substantially suppressed, leading to a transition to a nodal-line semiconducting state in CrCl3. These findings establish a diverse and highly tunable family of Q1D altermagnetic candidate materials.
Hanxiang Wu, Jianfeng Guo, Hua Xu, Zhaxi Suonan, Shuo Mi, Le Wang, Shanshan Chen, Rui Xu, Wei Ji, Zhihai Cheng, and Fei Pang*
Abstract:
2D non-van der Waals (vdW) Cr5Te8 has attracted widespread research interest for its air stability and thickness-dependent magnetic properties. However, the growth of large-scale ultrathin 2D Cr5Te8 remains challenging. Here, we selected GaTe powder as precursor to supply Te monomers and fabricated submillimeter 2D Cr5Te8 nanosheets. By optimizing the growth temperature and source–substrate distance (DSS), we successfully achieved Cr5Te8 nanosheets with lateral sizes of up to ~0.19 mm and corresponding thicknesses down to ~4.8 nm. The role of GaTe enhances the efficient Te atoms concentration, which promoted the lateral growth of Cr5Te8 nanosheets. Furthermore, our findings reveal the presence of Cr5Te8 nanosheets exhibiting serrated edges and a stacked structure like wedding cakes. Magnetic property measurement revealed the intense out-of-plane ferromagnetism in Cr5Te8, with the Curie temperature (TC) of 172 K. This work paves a way for the controllable growth of the submillimeter ultrathin 2D ferromagnetic crystalline and lays the foundation for the future synthesis of millimeter ultrathin ferromagnets.
Two-dimensional Janus materials exhibit unique physical properties due to broken inversional symmetries. However, it remains elusive to synthesize Janus monolayer crystals with tailored long-range magnetic orders. Here, we show a 2 ×√𝟑 charge density wave (CDW) transition and regulations of magnetization in a uniform Janus CrTeSe monolayer, selectively selenized from a pristine CrTe2 monolayer using molecular beam epitaxy. Scanning transmission electron microscopy images indicate the high quality and uniformity of the Janus structure. Spin-polarized scanning tunneling microscopy/spectroscopy measurements and density functional theory calculations unveil a robust zigzag antiferromagnetic order and the CDW transition in the CrTeSe monolayer. The one-side selenization breaks the vertical inversion symmetry, rotating the magnetic moment directions to the in-plane direction. The CDW transition opens a gap at the Fermi level and reorients the magnetic moments in tilted directions. Our work demonstrates the construction of large-area Janus structures and the tailoring of electronic and magnetic properties of two-dimensional Janus layers.
