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

Abstract

Since the celebrated discovery of graphene, the family of two-dimensional (2D) materials has grown to encompass a broad range of electronic properties. Recent additions include spin-valley coupled semiconductors, Ising superconductors that can be tuned into a quantum metal, possible Mott insulators with tunable charge-density waves, and topological semi-metals with edge transport. Despite this progress, there is still no 2D crystal with intrinsic magnetism, which would be useful for many technologies such as sensing, information, and data storage. Theoretically, magnetic order is prohibited in the 2D isotropic Heisenberg model at finite temperatures by the Mermin-Wagner theorem. However, magnetic anisotropy removes this restriction and enables, for instance, the occurrence of 2D Ising ferromagnetism. Here, we use magneto-optical Kerr effect (MOKE) microscopy to demonstrate that monolayer chromium triiodide (CrI 3) is an Ising ferromagnet with out-of-plane spin orientation. Its Curie temperature of 45 K is only slightly lower than the 61 K of the bulk crystal, consistent with a weak interlayer coupling. Moreover, our studies suggest a layer-dependent magnetic phases, showcasing the hallmark thickness dependent physical properties typical of van der Waals crystals. Remarkably, bilayer CrI3 displays suppressed magnetization with a metamagnetic effect, while in trilayer the interlayer ferromagnetism observed in the bulkmore » crystal is restored. Our work creates opportunities for studying magnetism by harnessing the unique features of atomically-thin materials, such as electrical control for realizing magnetoelectronics, and van der Waals engineering for novel interface phenomena.« less

Authors:
 [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)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Excitonics (CE)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1376527
Alternate Identifier(s):
OSTI ID: 1388215
Grant/Contract Number:  
AC05-00OR22725; SC0001088
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nature (London)
Additional Journal Information:
Journal Volume: 546; Journal Issue: 7657; Journal ID: ISSN 0028-0836
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Two-dimensional materials; polarization microscopy; solar (photovoltaic), solid state lighting, photosynthesis (natural and artificial), charge transport, optics, synthesis (novel materials), synthesis (self-assembly), synthesis (scalable processing)

Citation Formats

Huang, Bevin, Clark, Genevieve, Navarro-Moratalla, Efrén, Klein, Dahlia R., Cheng, Ran, Seyler, Kyle L., Zhong, Ding, Schmidgall, Emma, McGuire, Michael A., Cobden, David H., Yao, Wang, Xiao, Di, Jarillo-Herrero, Pablo, and Xu, Xiaodong. Layer-dependent ferromagnetism in a van der Waals crystal down to the monolayer limit. United States: N. p., 2017. Web. doi:10.1038/nature22391.
Huang, Bevin, Clark, Genevieve, Navarro-Moratalla, Efrén, Klein, Dahlia R., Cheng, Ran, Seyler, Kyle L., Zhong, Ding, Schmidgall, Emma, McGuire, Michael A., Cobden, David H., Yao, Wang, Xiao, Di, Jarillo-Herrero, Pablo, & Xu, Xiaodong. Layer-dependent ferromagnetism in a van der Waals crystal down to the monolayer limit. United States. doi:10.1038/nature22391.
Huang, Bevin, Clark, Genevieve, Navarro-Moratalla, Efrén, Klein, Dahlia R., Cheng, Ran, Seyler, Kyle L., Zhong, Ding, Schmidgall, Emma, McGuire, Michael A., Cobden, David H., Yao, Wang, Xiao, Di, Jarillo-Herrero, Pablo, and Xu, Xiaodong. Wed . "Layer-dependent ferromagnetism in a van der Waals crystal down to the monolayer limit". United States. doi:10.1038/nature22391. https://www.osti.gov/servlets/purl/1376527.
@article{osti_1376527,
title = {Layer-dependent ferromagnetism in a van der Waals crystal down to the monolayer limit},
author = {Huang, Bevin and Clark, Genevieve and Navarro-Moratalla, Efrén and Klein, Dahlia R. and Cheng, Ran and Seyler, Kyle L. and Zhong, Ding and Schmidgall, Emma and McGuire, Michael A. and Cobden, David H. and Yao, Wang and Xiao, Di and Jarillo-Herrero, Pablo and Xu, Xiaodong},
abstractNote = {Since the celebrated discovery of graphene, the family of two-dimensional (2D) materials has grown to encompass a broad range of electronic properties. Recent additions include spin-valley coupled semiconductors, Ising superconductors that can be tuned into a quantum metal, possible Mott insulators with tunable charge-density waves, and topological semi-metals with edge transport. Despite this progress, there is still no 2D crystal with intrinsic magnetism, which would be useful for many technologies such as sensing, information, and data storage. Theoretically, magnetic order is prohibited in the 2D isotropic Heisenberg model at finite temperatures by the Mermin-Wagner theorem. However, magnetic anisotropy removes this restriction and enables, for instance, the occurrence of 2D Ising ferromagnetism. Here, we use magneto-optical Kerr effect (MOKE) microscopy to demonstrate that monolayer chromium triiodide (CrI3) is an Ising ferromagnet with out-of-plane spin orientation. Its Curie temperature of 45 K is only slightly lower than the 61 K of the bulk crystal, consistent with a weak interlayer coupling. Moreover, our studies suggest a layer-dependent magnetic phases, showcasing the hallmark thickness dependent physical properties typical of van der Waals crystals. Remarkably, bilayer CrI3 displays suppressed magnetization with a metamagnetic effect, while in trilayer the interlayer ferromagnetism observed in the bulk crystal is restored. Our work creates opportunities for studying magnetism by harnessing the unique features of atomically-thin materials, such as electrical control for realizing magnetoelectronics, and van der Waals engineering for novel interface phenomena.},
doi = {10.1038/nature22391},
journal = {Nature (London)},
issn = {0028-0836},
number = 7657,
volume = 546,
place = {United States},
year = {2017},
month = {6}
}

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