Crystal Growth, Exfoliation and Magnetic Properties of Quaternary Quasi-Two-Dimensional CuCrP$_2$S$_6$

Abstract: We report optimized crystal growth conditions for the quaternary compound CuCrP$2$S$_6$ by chemical vapor transport. Compositional and structural characterization of the obtained crystals were carried out by means of energy-dispersive X-ray spectroscopy and powder X-ray diffraction. CuCrP$_2$S$_6$ is structurally closely related to the $M_2$P$_2$S$_6$ family ($M$: transition metal), which contains several compounds that are under investigation as 2D magnets. As-grown crystals exhibit a plate-like, layered morphology as well as a hexagonal habitus. We present successful exfoliation of such as-grown crystals down to thicknesses of 2.8 nm corresponding to 4 layers. CuCrP$_2$S$_6$ crystallizes in the monoclinic space group $C2/c$. Magnetization measurements reveal an antiferromagnetic ground state with $T\textrm{N} \approx 30$ K and a positive Curie-Weiss temperature in agreement with dominant ferromagnetic intralayer coupling. Specific heat measurements confirm this magnetic phase transition and the magnetic order is suppressed in an external magnetic field of about 6 T (8 T) applied parallel (perpendicular) to the $ab$ plane. At higher temperatures between 140-200 K additional broad anomalies associated with structural changes accompanying antiferroelectric ordering are detected in our specific heat studies.