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CrCl3 is a layered insulator that undergoes a crystallographic phasetransition below room temperature and orders antiferromagnetically at lowtemperature. Weak van der Waals bonding between the layers and ferromagneticin-plane magnetic order make it a promising material for obtaining atomicallythin magnets and creating van der Waals heterostructures. In this work we havegrown crystals of CrCl3, revisited the structural and thermodynamic propertiesof the bulk material, and explored mechanical exfoliation of the crystals. Wefind two distinct anomalies in the heat capacity at 14 and 17 K confirming thatthe magnetic order develops in two stages on cooling, with ferromagneticcorrelations forming before long range antiferromagnetic order develops betweenthem. This scenario is supported by magnetization data. A magnetic phasediagram is constructed from the heat capacity and magnetization results. Wealso find an anomaly in the magnetic susceptibility at the crystallographicphase transition, indicating some coupling between the magnetism and thelattice. First principles calculations accounting for van der Waalsinteractions also indicate spin-lattice coupling, and find multiple nearlydegenerate crystallographic and magnetic structures consistent with theexperimental observations. Finally, we demonstrate that monolayer and few-layerCrCl3 specimens can be produced from the bulk crystals by exfoliation,providing a path for the study of heterostructures and magnetism in ultrathincrystals down to the monolayer limit.

Magnetic Behavior and Spin-Lattice Coupling in Cleavable, van der Waals Layered CrCl3 Crystals