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.
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.
Deping Guo (郭的坪)#, Cong Wang (王聪)#, Lvjin Wang (王侣锦), Yunhao Lu (陆赟豪), Hua Wu (吴骅), Yanning Zhang (张妍宁), and Wei Ji (季威)*
Abstract:
Two-dimensional (2D) van der Waals magnetic materials have promising and versatile electronic and magnetic properties in the 2D limit, indicating a considerable potential to advance spintronic applications. Theoretical predictions thus far have not ascertained whether monolayer VCl3 is a ferromagnetic (FM) or anti-FM monolayer; this also remains to be experimentally verified. We theoretically investigate the influence of potential factors, including 𝐶3 symmetry breaking, orbital ordering, epitaxial strain, and charge doping, on the magnetic ground state. Utilizing first-principles calculations, we predict a collinear type-III FM ground state in monolayer VCl3 with a broken 𝐶3 symmetry, wherein only the former two of three 𝑡2g orbitals (𝑎1g, 𝑒 𝜋 g2 and 𝑒 𝜋 g1) are occupied. The atomic layer thickness and bond angles of monolayer VCl3 undergo abrupt changes driven by an orbital ordering switch, resulting in concomitant structural and magnetic phase transitions. Introducing doping to the underlying Cl atoms of monolayer VCl3 without 𝐶3 symmetry simultaneously induces in- and out-of-plane polarizations. This can achieve a multiferroic phase transition if combined with the discovered adjustments of magnetic ground state and polarization magnitude under strain. The establishment of an orbital-ordering driven regulatory mechanism can facilitate deeper exploration and comprehension of magnetic properties of strongly correlated systems in monolayer VCl3.
The quest for pragmatic room-temperature (RT) magnetic semiconductors (MSs) with a suitable bandgap constitutes one of the contemporary opportunities to be exploited. This may provide a materials platform for to bring new-generation ideal information device technologies into real-world applications where the otherwise conventionally separately utilized charge and spin are simultaneously exploited. Here we present RT ferromagnetism in an Fe-doped SnSe (Fe:SnSe) van der Waals (vdW) single crystalline ferromagnetic semiconductor (FMS) with a semiconducting bandgap of ∼1.19 eV (comparable to those of Si and GaAs). The synthesized Fe:SnSe single crystals feature a dilute Fe content of <1.0 at%, a Curie temperature of ∼310 K, a layered vdW structure nearly identical to that of pristine SnSe, and the absence of in-gap defect states. The Fe:SnSe vdW diluted magnetic semiconductor (DMS) single crystals are grown using a simple temperature-gradient melt-growth process, in which the magnetic Fe atom doping is realized uniquely using FeI2 as the dopant precursor whose melting point is low with respect to crystal growth, and which in principle possesses industrially unlimited scalability. Our work adds a new member in the family of long-searching RT magnetic semiconductors, and may establish a generalized strategy for large-volume production of related DMSs.
