Hanxiang Wu, Zuoquan Tan, Zhaxi Suonan, Shanshan Chen, Rui Xu, Wei Ji, Zhihai Cheng, and Fei Pang*
Abstract:
Although 2D self-intercalated Cr5Te8 has been successfully synthesized via chemical vapor deposition (CVD), its etching behavior remains largely unexplored. Etching, as the inverse process of material growth, is essential for understanding growth mechanisms and fabricating nanosheet patterns. Herein, we explore the anisotropic etching of 2D Cr5Te8 assisted by an excess Te supply. The etching process initiates from both the surface and the edge, creating distinct holes and nanoribbons with triangular or hexagonal shapes. To the best of our knowledge, this is the first report on controllable anisotropic etching patterns in 2D Cr5Te8. Furthermore, magnetic measurements reveal ferromagnetism in the etched nanosheets with a Curie temperature (TC) of 164 K, slightly lower than that of the unetched nanosheets. The etched nanosheets exhibit an enhanced saturated magnetic field of 38.5 kOe, approximately 3.2 times that of the unetched nanosheets. This enhancement in the saturated magnetic field is attributed to the pattern-induced strengthening of the reentrant stray field. This study offers a new direction for preparing patterned 2D materials and opens a novel avenue for modulating 2D magnetism.
Altermagnetism has recently drawn considerable attention in three- and two-dimensional materials. Here we extend this concept to quasi-one-dimensional (Q1D) monolayers assembled from single-atomic magnetic chains. Through systematically examining nine types of structures, two stacking orders, intra- and interchain magnetic couplings, we identify four out of 30 promising structural prototypes for hosting altermagnetism, which yields 192 potential monolayer materials. We further confirm eight thermodynamically stable Q1D monolayers via high-throughput calculations. Using symmetry analysis and first-principles calculations, we find that the existence of altermagnetism is determined by the type of interchain magnetic coupling and predict three intrinsic altermagnets, CrBr3, VBr3, and MnBr3, due to their ferromagnetic interchain couplings and five extrinsic ones, CrF3, CrCl3, CrI3, FeCl3, and CoTe3, ascribed to their neglectable or antiferromagnetic interchain couplings. Moreover, the interchain magnetic coupling here is highly tunable by manipulating the interchain spacing, leading to experimentally feasible transitions between altermagnetic and nodal-line semiconducting states. In addition, applying external electric fields can further modulate the spin splitting. Our findings establish a highly tunable family of Q1D altermagnets, offering fundamental insights into the intricate relationship between geometry, electronic structure, and magnetism. These discoveries hold significant promises for experimental realization and future spintronic applications.
FIG. 1. (a) Summary of the emergence of altermagnetism in 1D magnetic chains with different stoichiometric ratios under AA and AB stacking configurations. FM and AFM represent interchain magnetic ordering. The symbol “×” indicates the absence of altermagnetism, while “ ” signifies its emergence. The symbol “/” represents the absence of the AB stacking configuration. Top (upper panel) and side (lower panel) views of the AA-stacked (b) and AB-stacked (c) γ -phase XY2 (X = transition metal, Y = chalcogen/halogen atom) and AA-stacked (d) and AB-stacked (e) β-phase XY3 monolayers. Orange arrows and blue lines illustrate symmetry operations C2x and Mx that connect the sublattices with opposite spins. Red dots P1 to P3 marked in panel (d) indicate structural inversion centers. Orange and blue spheres represent magnetic atoms with up and down majority spins, respectively. J1, J2, and J3 marked in panel (e) represent spin-exchange parameters for the nearest, second-nearest, and third-nearest neighbors, respectively. (f) Diagram of spin-splitting symmetry in the Brillouin zone.
FIG. 2. (a) The screening process of Q1D altermagnets. (b) Top view of spin density distribution and (c) band structure of the CrCl3 monolayer at the interchain spacing of 6.0 Å. The red dot represents the inversion center. The illustration shows the high-symmetry path in the Brillouin zone. (d), (e) The same scheme of (b), (c) for the CrCl3 monolayer with an expanded interchain spacing of 6.40 Å. The red dashed box highlights nodal-line electronic states.
TABLE I. Lattice constants (a and b) and spin-exchange parameters [J1, J2, J3, labeled in Fig. 1(e), in units of meV per magnetic atom] of the eight dynamically stable AA-stacked intrachain AFM β-XY3 Q1D monolayers.
FIG. 3. (a) The energy difference (EAFM -EFM ) as a function of interchain spacing for Q1D VBr3 monolayer. The vertical dashed line indicates the freestanding interchain distance. (b) Band structure of the monolayer VBr3 under interchain of 6.80 Å [labeled as red pentagram in 3(a)]. (c) The energy difference as a function of interchain spacing for Q1D CoTe3 monolayer. (d) Band structure of the monolayer CoTe3 under interchain of 5.10 Å [labeled as red pentagram in 3(c)].
FIG. 4. (a) Band dispersion plots of the highest valence band in freestanding CrCl3 monolayer with interchain FM coupling under varied external electric field. The orange dots indicate the band crossing point along the -S direction. Spin splitting mappings of the highest valence band in the freestanding CrCl3 monolayer (b) without electric field and (c) under an electric field of 0.2 V/Å.
As a fundamental structural feature, the symmetry of materials determines the exotic quantum properties in transition metal dichalcogenides (TMDs) with charge density waves (CDWs). The Janus structure, an artificially constructed lattice, provides an opportunity to tune the electronic structures and their associated behavior, such as CDW states. However, limited by the difficulties in atomic-level fabrication and material stability, the experimental visualization of the CDW states in two-dimensional (2D) TMDs with Janus structure is still rare. Here, using surface selenization of VTe2, we fabricated monolayer Janus VTeSe. With scanning tunneling microscopy, we observed and characterized an unusual sqrt13 x sqrt13 CDW state with threefold rotational symmetry breaking. Combined with theoretical calculations, we find that this CDW state can be attributed to the magnetic-involved charge modulation in the Janus VTeSe, rather than the conventional electron-phonon coupling. Our findings provide a promising platform for studying the CDW states and artificially tuning the electronic properties of the 2D TMDs toward the related fundamental and applied studies.
Two-dimensional (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 the 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 a lateral size of up to ∼0.19 mm and corresponding thickness down to ∼4.8 nm. The role of GaTe is to enhance the efficient Te atom concentration, which promotes the lateral growth of Cr5Te8 nanosheets. Furthermore, our findings reveal the appearance of Cr5Te8 nanosheets exhibiting serrated edges and a stacked structure like those of wedding cakes. Magnetic property measurement revealed the intense out-of-plane ferromagnetism in Cr5Te8, with a Curie temperature (TC) of 172 K. This work paves the way for the controllable growth of submillimeter ultrathin 2D ferromagnetic crystals and lays the foundation for the future synthesis of millimeter ultrathin ferromagnets.
Wenjuan Zhao#, Xieyu Zhou#, Dayu Yan#, Yuan Huang*, Cong Li, Qiang Gao, Paolo Moras, Polina M. Sheverdyaeva, Hongtao Rong, Yongqing Cai, Eike F. Schwier, Xixia Zhang, Cheng Shen, Yang Wang, Yu Xu, Wei Ji, Chen Liu, Youguo Shi, Lin Zhao, Lihong Bao, Qingyan Wang, Kenya Shimada, Xutang Tao, Guangyu Zhang, Hongjun Gao, Zuyan Xu, Xingjiang Zhou*, Guodong Liu*
Abstract:
An in-depth understanding of the electronic structure of 2H-MoTe2 at the atomic layer limit is a crucial step towards its exploitation in nanoscale devices. Here, we show that millimeter-sized monolayer (ML) MoTe2 samples, as well as smaller sized bilayer (BL) samples, can be obtained using the mechanical exfoliation technique. The electronic structure of these materials is investigated by Angle-Resolved Photoemission Spectroscopy (ARPES) for the first time and Density Functional Theory (DFT) calculations. The comparison between experiments and theory allows us to describe ML MoTe2 as a semiconductor with direct gap at K point. This scenario is reinforced by the experimental observation of the conduction band minimum at K in Rb-doped ML MoTe2, resulting in a gap of at least 0.924 eV. In the BL MoTe2 system the maxima of the bands at Γ and K display very similar energies, thus leaving the door open to a direct gap scenario, in analogy to WSe2. The monotonic increase in the separation between spin-split bands at K while moving from ML to BL and bulk-like MoTe2 is attributed to interlayer coupling. Our findings can be considered as a reference to understand Quantum Anomalous and Fractional Quantum Anomalous Hall Effects recently discovered in ML and BL MoTe2 based moir´ e heterostructures.
