skip to main content

Title: Intrinsic ferromagnetism and topological properties in two-dimensional rhenium halides
The realization of robust intrinsic ferromagnetism in two-dimensional (2D) materials in conjunction with the intriguing quantum anomalous Hall (QAH) effect has provided a fertile ground for novel physics and for the next-generation spintronic and topological devices. On the basis of density functional theory (DFT), we predict that layered 5d transition-metal heavier halides (TMHs), such as ReX 3 (X = Br, I), show intrinsic ferromagnetism with high spin polarization and high Curie temperatures. The outstanding dynamic and thermodynamic stability ensures their experimental feasibility. The strong spin–orbit coupling (SOC) of Re makes the electronic structure of the ReI 3 monolayer topologically nontrivial with a large Chern number ( C = −4). DFT+ U calculations reveal that the 2D system undergoes a nontrivial to trivial transition with increasing on-site Hubbard Coulomb interaction U through the emergence of a Dirac cone. This transition is corroborated by the emergence of chiral edge states and the anomalous Hall conductivity. These findings not only demonstrate room-temperature ferromagnetism in atomically thin 5d TMHs, but also pave the way for the potential realization of the QAH effect with high Chern numbers in pristine 2D layers.
Authors:
;
Award ID(s):
1828019
Publication Date:
NSF-PAR ID:
10104174
Journal Name:
Nanoscale
Volume:
11
Issue:
13
Page Range or eLocation-ID:
6101 to 6107
ISSN:
2040-3364
Sponsoring Org:
National Science Foundation
More Like this
  1. A major recent breakthrough in materials science is the emergence of intrinsic magnetism in two-dimensional (2D) crystals, which opens the door to more cutting-edge fields in the 2D family and could eventually lead to novel data-storage and information devices with further miniaturization. Herein we propose an experimentally feasible 2D material, Fe 2 I 2 , which is an intrinsic room-temperature ferromagnet exhibiting perpendicular magnetic anisotropy (PMA). Using first-principles calculations, we demonstrate that single-layer (SL) Fe 2 I 2 is a spin-gapless semiconductor with a spin-polarized Dirac cone and linear energy dispersion in one spin channel, exhibiting promising dissipation-less transport properties with a Fermi velocity up to 6.39 × 10 5 m s −1 . Our results reveal that both strain and ferroelectric polarization switching could induce an out-of- to in-plane spin reorientation in the 2D Fe 2 I 2 layer, revealing its advantage in assembling spintronic devices. In addition, spin–orbit coupling (SOC) triggers a topologically nontrivial band gap of 301 meV with a nonzero Chern number (| C | = 2), giving rise to a robust quantum anomalous Hall (QAH) state. The 2D crystal also exhibits high carrier mobilites of 0.452 × 10 3 and 0.201 × 10 3 cmmore »2 V −1 s −1 for the electrons and holes, respectively. The combination of these unique properties renders the 2D Fe 2 I 2 ferromagnet a promising platform for high efficiency multi-functional spintronic applications.« less
  2. Abstract

    The physical realization of Chern insulators is of fundamental and practical interest, as they are predicted to host the quantum anomalous Hall (QAH) effect and topologically protected chiral edge states which can carry dissipationless current. Current realizations of the QAH state often require complex heterostructures and sub-Kelvin temperatures, making the discovery of intrinsic, high temperature QAH systems of significant interest. In this work we show that time-reversal symmetry breaking Weyl semimetals, being essentially stacks of Chern insulators with inter-layer coupling, may provide a new platform for the higher temperature realization of robust chiral edge states. We present combined scanning tunneling spectroscopy and theoretical investigations of the magnetic Weyl semimetal, Co3Sn2S2. Using modeling and numerical simulations we find that depending on the strength of the interlayer coupling, chiral edge states can be localized on partially exposed kagome planes on the surfaces of a Weyl semimetal. Correspondingly, our dI/dVmaps on the kagome Co3Sn terraces show topological states confined to the edges which display linear dispersion. This work provides a new paradigm for realizing chiral edge modes and provides a pathway for the realization of higher temperature QAH effect in magnetic Weyl systems in the two-dimensional limit.

  3. Abstract MnBi 2 Te 4 /(Bi 2 Te 3 ) n materials system has recently generated strong interest as a natural platform for the realization of the quantum anomalous Hall (QAH) state. The system is magnetically much better ordered than substitutionally doped materials, however, the detrimental effects of certain disorders are becoming increasingly acknowledged. Here, from compiling structural, compositional, and magnetic metrics of disorder in ferromagnetic (FM) MnBi 2 Te 4 /(Bi 2 Te 3 ) n it is found that migration of Mn between MnBi 2 Te 4 septuple layers (SLs) and otherwise non-magnetic Bi 2 Te 3 quintuple layers (QLs) has systemic consequences—it induces FM coupling of Mn-depleted SLs with Mn-doped QLs, seen in ferromagnetic resonance as an acoustic and optical resonance mode of the two coupled spin subsystems. Even for a large SL separation ( n ≳ 4 QLs) the structure cannot be considered as a stack of uncoupled two-dimensional layers. Angle-resolved photoemission spectroscopy and density functional theory studies show that Mn disorder within an SL causes delocalization of electron wave functions and a change of the surface band structure as compared to the ideal MnBi 2 Te 4 /(Bi 2 Te 3 ) n . Thesemore »findings highlight the critical importance of inter- and intra-SL disorder towards achieving new QAH platforms as well as exploring novel axion physics in intrinsic topological magnets.« less
  4. Abstract

    The emergence of ferromagnetism in materials where the bulk phase does not show any magnetic order demonstrates that atomically precise films can stabilize distinct ground states and expands the phase space for the discovery of materials. Here, the emergence of long-range magnetic order is reported in ultrathin (111) LaNiO3(LNO) films, where bulk LNO is paramagnetic, and the origins of this phase are explained. Transport and structural studies of LNO(111) films indicate that NiO6octahedral distortions stabilize a magnetic insulating phase at the film/substrate interface and result in a thickness-dependent metal–insulator transition att = 8 unit cells. Away from this interface, distortions relax and bulk-like conduction is regained. Synchrotron x-ray diffraction and dynamical x-ray diffraction simulations confirm a corresponding out-of-plane unit-cell expansion at the interface of all films. X-ray absorption spectroscopy reveals that distortion stabilizes an increased concentration of Ni2+ions. Evidence of long-range magnetic order is found in anomalous Hall effect and magnetoresistance measurements, likely due to ferromagnetic superexchange interactions among Ni2+–Ni3+ions. Together, these results indicate that long-range magnetic ordering and metallicity in LNO(111) films emerges from a balance among the spin, charge, lattice, and orbital degrees of freedom.

  5. Abstract

    Co$$_{3}$$3Sn$$_{2}$$2S$$_{2}$$2is a ferromagnetic Weyl semimetal that has been the subject of intense scientific interest due to its large anomalous Hall effect. We show that the coupling of this material’s topological properties to its magnetic texture leads to a strongly exchange biased anomalous Hall effect. We argue that this is likely caused by the coexistence of ferromagnetism and geometric frustration intrinsic to the kagome network of magnetic ions, giving rise to spin-glass behavior and an exchange bias.