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Coupling of Crystal Structure and Magnetism in the Layered, Ferromagnetic Insulator CrI3
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    Coupling of Crystal Structure and Magnetism in the Layered, Ferromagnetic Insulator CrI3
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    Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee United States
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    Chemistry of Materials

    Cite this: Chem. Mater. 2015, 27, 2, 612–620
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    https://doi.org/10.1021/cm504242t
    Published December 23, 2014
    Copyright © 2014 American Chemical Society

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    We have examined the crystallographic and magnetic properties of single crystals of CrI3, an easily cleavable, layered and insulating ferromagnet with a Curie temperature of 61 K. Our X-ray diffraction studies reveal a first-order crystallographic phase transition occurring near 210–220 K upon warming, with significant thermal hysteresis. The low-temperature structure is rhombohedral (R3̅, BiI3-type) and the high-temperature structure is monoclinic (C2/m, AlCl3-type). We find evidence for coupling between the crystallographic and magnetic degrees of freedom in CrI3, observing an anomaly in the interlayer spacing at the Curie temperature and an anomaly in the magnetic susceptibility at the structural transition. First-principles calculations reveal the importance of proper treatment of the long-ranged interlayer forces, and van der Waals density functional theory does an excellent job of predicting the crystal structures and their relative stability. Calculations also suggest that the ferromagnetic order found in the bulk material may persist into monolayer form, suggesting that CrI3 and other chromium trihalides may be promising materials for spintronic and magnetoelectronic research.

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    Description of the disorder model used for the low-temperature structural refinements, comparison of structures determined here with a previously reported structural model in space group P3112, and electronic band structures, DOSs, and binding energy curves from density functional theory calculations. This material is available free of charge via the Internet at http://pubs.acs.org.

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    Cite this: Chem. Mater. 2015, 27, 2, 612–620
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    Published December 23, 2014
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