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Title: Magnetic behavior and spin-lattice coupling in cleavable van der Waals layered CrCl 3 crystals

CrCl 3 is a layered insulator that undergoes a crystallographic phase transition below room temperature and orders antiferromagnetically at low temperature. Weak van der Waals bonding between the layers and ferromagnetic in-plane magnetic order make it a promising material for obtaining atomically thin magnets and creating van der Waals heterostructures. In this work we have grown crystals of CrCl 3, revisited the structural and thermodynamic properties of the bulk material, and explored mechanical exfoliation of the crystals. We find two distinct anomalies in the heat capacity at 14 and 17 K confirming that the magnetic order develops in two stages on cooling, with ferromagnetic correlations forming before long-range antiferromagnetic order develops between them. This scenario is supported by magnetization data. A magnetic phase diagram is constructed from the heat capacity and magnetization results. We also find an anomaly in the magnetic susceptibility at the crystallographic phase transition, indicating some coupling between the magnetism and the lattice. First-principles calculations accounting for van der Waals interactions also indicate spin-lattice coupling, and find multiple nearly degenerate crystallographic and magnetic structures consistent with the experimental observations. Lastly, we demonstrate that monolayer and few-layer CrCl 3 specimens can be produced from the bulk crystals bymore » exfoliation, providing a path for the study of heterostructures and magnetism in ultrathin crystals down to the monolayer limit.« less
Authors:
 [1] ;  [2] ; ORCiD logo [1] ;  [3] ;  [1] ;  [1] ;  [2] ;  [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Univ. of Washington, Seattle, WA (United States)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); The Univ. of Tennessee, Knoxville, TN (United States)
Publication Date:
Grant/Contract Number:
AC05-00OR22725; AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
Physical Review Materials
Additional Journal Information:
Journal Volume: 1; Journal Issue: 1; Journal ID: ISSN 2475-9953
Publisher:
American Physical Society (APS)
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE
OSTI Identifier:
1376459
Alternate Identifier(s):
OSTI ID: 1364213; OSTI ID: 1376530

McGuire, Michael A., Clark, Genevieve, KC, Santosh, Chance, W. Michael, Jellison, Jr., Gerald E., Cooper, Valentino R., Xu, Xiaodong, and Sales, Brian C.. Magnetic behavior and spin-lattice coupling in cleavable van der Waals layered CrCl3 crystals. United States: N. p., Web. doi:10.1103/PhysRevMaterials.1.014001.
McGuire, Michael A., Clark, Genevieve, KC, Santosh, Chance, W. Michael, Jellison, Jr., Gerald E., Cooper, Valentino R., Xu, Xiaodong, & Sales, Brian C.. Magnetic behavior and spin-lattice coupling in cleavable van der Waals layered CrCl3 crystals. United States. doi:10.1103/PhysRevMaterials.1.014001.
McGuire, Michael A., Clark, Genevieve, KC, Santosh, Chance, W. Michael, Jellison, Jr., Gerald E., Cooper, Valentino R., Xu, Xiaodong, and Sales, Brian C.. 2017. "Magnetic behavior and spin-lattice coupling in cleavable van der Waals layered CrCl3 crystals". United States. doi:10.1103/PhysRevMaterials.1.014001. https://www.osti.gov/servlets/purl/1376459.
@article{osti_1376459,
title = {Magnetic behavior and spin-lattice coupling in cleavable van der Waals layered CrCl3 crystals},
author = {McGuire, Michael A. and Clark, Genevieve and KC, Santosh and Chance, W. Michael and Jellison, Jr., Gerald E. and Cooper, Valentino R. and Xu, Xiaodong and Sales, Brian C.},
abstractNote = {CrCl3 is a layered insulator that undergoes a crystallographic phase transition below room temperature and orders antiferromagnetically at low temperature. Weak van der Waals bonding between the layers and ferromagnetic in-plane magnetic order make it a promising material for obtaining atomically thin magnets and creating van der Waals heterostructures. In this work we have grown crystals of CrCl3, revisited the structural and thermodynamic properties of the bulk material, and explored mechanical exfoliation of the crystals. We find two distinct anomalies in the heat capacity at 14 and 17 K confirming that the magnetic order develops in two stages on cooling, with ferromagnetic correlations forming before long-range antiferromagnetic order develops between them. This scenario is supported by magnetization data. A magnetic phase diagram is constructed from the heat capacity and magnetization results. We also find an anomaly in the magnetic susceptibility at the crystallographic phase transition, indicating some coupling between the magnetism and the lattice. First-principles calculations accounting for van der Waals interactions also indicate spin-lattice coupling, and find multiple nearly degenerate crystallographic and magnetic structures consistent with the experimental observations. Lastly, we demonstrate that monolayer and few-layer CrCl3 specimens can be produced from the bulk crystals by exfoliation, providing a path for the study of heterostructures and magnetism in ultrathin crystals down to the monolayer limit.},
doi = {10.1103/PhysRevMaterials.1.014001},
journal = {Physical Review Materials},
number = 1,
volume = 1,
place = {United States},
year = {2017},
month = {6}
}

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