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Title: Layer-dependent ferromagnetism in a van der Waals crystal down to the monolayer limit

Journal Article · · Nature (London)
DOI:https://doi.org/10.1038/nature22391· OSTI ID:1376527
 [1];  [1];  [2];  [2];  [3];  [1];  [1];  [1];  [4];  [1];  [5];  [3];  [2];  [1]
  1. Univ. of Washington, Seattle, WA (United States)
  2. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  3. Carnegie Mellon Univ., Pittsburgh, PA (United States)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  5. Univ. of Hong Kong (China)

Since the discovery of graphene, the family of two-dimensional materials has grown, displaying a broad range of electronic properties. Recent additions include semiconductors with spin–valley coupling, Ising superconductors that can be tuned into a quantum metal, possible Mott insulators with tunable charge-density waves, and topological semimetals with edge transport. However, no two-dimensional crystal with intrinsic magnetism has yet been discovered; such a crystal would be useful in many technologies from sensing to data storage. Theoretically, magnetic order is prohibited in the two-dimensional isotropic Heisenberg model at finite temperatures by the Mermin–Wagner theorem. Magnetic anisotropy removes this restriction, however, and enables, for instance, the occurrence of two-dimensional Ising ferromagnetism. Here we use magneto-optical Kerr effect microscopy to demonstrate that monolayer chromium triiodide (CrI3) is an Ising ferromagnet with out-of-plane spin orientation. Its Curie temperature of 45 kelvin is only slightly lower than that of the bulk crystal, 61 kelvin, which is consistent with a weak interlayer coupling. Moreover, our studies suggest a layer-dependent magnetic phase, highlighting thickness-dependent physical properties typical of van der Waals crystals. Remarkably, bilayer CrI3 displays suppressed magnetization with a metamagnetic effect, whereas in trilayer CrI3 the interlayer ferromagnetism observed in the bulk crystal is restored. This work creates opportunities for studying magnetism by harnessing the unusual features of atomically thin materials, such as electrical control for realizing magnetoelectronics, and van der Waals engineering to produce interface phenomena.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Excitonics (CE)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC05-00OR22725; SC0001088
OSTI ID:
1376527
Alternate ID(s):
OSTI ID: 1388215
Journal Information:
Nature (London), Vol. 546, Issue 7657; ISSN 0028-0836
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 3395 works
Citation information provided by
Web of Science

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2DMatPedia, an open computational database of two-dimensional materials from top-down and bottom-up approaches journal June 2019
Interference induced enhancement of magneto-optical Kerr effect in ultrathin magnetic films journal January 2018
Dirac cone intensity asymmetry and surface magnetic field in V-doped and pristine topological insulators generated by synchrotron and laser radiation journal April 2018
Dirac gap opening and Dirac-fermion-mediated magnetic coupling in antiferromagnetic Gd-doped topological insulators and their manipulation by synchrotron radiation journal March 2019
Proximity-Induced Artefacts in Magnetic Imaging with Nitrogen-Vacancy Ensembles in Diamond journal April 2018
Very large tunneling magnetoresistance in layered magnetic semiconductor CrI3 text January 2018
Mixed topological semimetals driven by orbital complexity in two-dimensional ferromagnets text January 2018
Asymmetric dynamics of edge exchange spin waves in honeycomb nanoribbons with zigzag and bearded edges boundaries text January 2019
Suppression of magnetic ordering in XXZ-type antiferromagnetic monolayer NiPS3 text January 2019
Giant Valley Splitting in Monolayer WS2 by Magnetic Proximity Effect text January 2019