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Magnetic behavior and spin-lattice coupling in cleavable, van der Waals layered CrCl3 crystals
Physical Review Materials (2017)
  • Michael A. McGuire, Oak Ridge National Laboratory
  • Genevieve Clark, University of Washington
  • Santosh KC, Oak Ridge National Laboratory
  • W. Michael Chance, Oak Ridge National Laboratory
  • Gerald E. Jellison, Jr., Oak Ridge National Laboratory
  • Valentino R. Cooper, Oak Ridge National Laboratory
  • Xiaodong Xu, University of Washington
  • Brian C. Sales, Oak Ridge National Laboratory
Abstract
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. Finally, 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.
Publication Date
June 19, 2017
DOI
10.1103/PhysRevMaterials.1.014001
Publisher Statement
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This article was published in Physical Review Materials, volume 1, issue 1, 2017, and can also be found online here.
©2017 American Physical Society
Citation Information
Michael A. McGuire, Genevieve Clark, Santosh KC, W. Michael Chance, et al.. "Magnetic behavior and spin-lattice coupling in cleavable, van der Waals layered CrCl3 crystals" Physical Review Materials Vol. 1 Iss. 1 (2017)
Available at: http://works.bepress.com/santosh-kc/13/