Incommensurate antiferromagnetic order in weakly frustrated two-dimensional van der Waals insulator CrPSe$_3$

Abstract: Although the magnetic order is suppressed by a strong magnetic frustration, it is maintained but appears in complex order forms such as a cycloid or spin density wave in weakly frustrated systems. Herein, we report a weakly magnetic-frustrated two-dimensional van der Waals material CrPSe$3$. Polycrystalline CrPSe$_3$ was synthesized at an optimized temperature of 700$^\circ$C to avoid the formation of any secondary phases (e.g., Cr$_2$Se$_3$). The antiferromagnetic transition appeared at $T_N\sim 126$ K with a large Curie-Weiss temperature $T{\rm CW} \sim -371$ via magnetic susceptibility measurements, indicating weak frustration in CrPSe$3$ with a frustration factor $f (|T{\rm CW}|/T_N) \sim 3$. Evidently, the formation of long-range incommensurate spin-density wave antiferromagnetic order with the propagation vector $k = (0, 0.04, 0)$ was revealed by neutron diffraction measurements at low temperatures (below 120K). The monoclinic crystal structure of C2/m symmetry is preserved over the studied temperature range down to 20K, as confirmed by Raman spectroscopy measurements. Our findings on the spin density wave antiferromagnetic order in two-dimensional (2D) magnetic materials, not previously observed in the MPX$_3$ family, are expected to enrich the physics of magnetism at the 2D limit, thereby opening opportunities for their practical applications in spintronics and quantum devices.