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.
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This content will become publicly available on May 3, 2024
New insights into band inversion and topological phase of TiNI monolayer
Two-dimensional (2D) topological insulators (TIs) hold great promise for future quantum information technologies. Among the 2D-TIs, the TiNI monolayer has recently been proposed as an ideal material for achieving the quantum spin Hall effect at room temperature. Theoretical predictions suggest a sizable bandgap due to the spin–orbit coupling (SOC) of the electrons at and near the Fermi level with a nontrivial 2 topology of the electronic states, which is robust under external strain. However, our detailed first-principles calculations reveal that, in contrast to these predictions, the TiNI monolayer has a trivial bandgap in the equilibrium state with no band inversion, despite SOC opening the bandgap. Moreover, we show that electron correlation effects significantly impact the topological and structural stabilities of the system under external strains. We employed a range of density functional theory (DFT) approaches, including HSE06, PBE0, TB-mBJ, and GGA+ U , to comprehensively investigate the nontrivial topological properties of this monolayer. Our results demonstrate that using general-purpose functionals such as PBE-GGA for studying TIs can lead to false predictions, potentially misleading experimentalists in their efforts to discover new TIs.
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- Award ID(s):
- 2110603
- NSF-PAR ID:
- 10443224
- Date Published:
- Journal Name:
- Physical Chemistry Chemical Physics
- Volume:
- 25
- Issue:
- 17
- ISSN:
- 1463-9076
- Page Range / eLocation ID:
- 12182 to 12191
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract Magnetic skyrmions are topologically nontrivial chiral spin textures that have potential applications in next‐generation energy‐efficient and high‐density spintronic devices. In general, the chiral spins of skyrmions are stabilized by the noncollinear Dzyaloshinskii–Moriya interaction (DMI), originating from the inversion symmetry breaking combined with the strong spin–orbit coupling (SOC). Here, the strong SOC from topological insulators (TIs) is utilized to provide a large interfacial DMI in TI/ferrimagnet heterostructures at room temperature, resulting in small‐size (radius ≈ 100 nm) skyrmions in the adjacent ferrimagnet. Antiferromagnetically coupled skyrmion sublattices are observed in the ferrimagnet by element‐resolved scanning transmission X‐ray microscopy, showing the potential of a vanishing skyrmion Hall effect and ultrafast skyrmion dynamics. The line‐scan spin profile of the single skyrmion shows a Néel‐type domain wall structure and a 120 nm size of the 180° domain wall. This work demonstrates the sizable DMI and small skyrmions in TI‐based heterostructures with great promise for low‐energy spintronic devices.
