Controlling Spin Orientation and Metamagnetic Transitions in Anisotropic van der Waals Antiferromagnet CrPS₄ by Hydrostatic Pressure

Abstract

Controlling the phases of matter is a central task in condensed matter physics and materials science. In 2D magnets, manipulating spin orientation is of great significance in the context of the Mermin-Wagner theorem. Herein, a systematic study of temperature-and pressure-dependent magnetic properties up to 1 GPa in van der Waals CrPS 4 is reported. Owing to the temperature-dependent change of the magnetic anisotropy energy, the material undergoes a first-order spin reorientation transition with magnetic moments realigning from being almost parallel with the c axis in the ac plane to the quasi-1D chains of CrS 6 octahedra along the b axis upon heating. The spin reorientation temperature is suppressed after applying pressure, shifting the high-temperature phase to lower temperatures with the emergence of spinflop transitions under magnetic fields applied along the b axis. The saturation field increases with pressure, indicating the enhancement of interlayer antiferromagnetic coupling. However, the Néel temperature is slightly reduced, which is ascribed to the suppression of intralayer ferromagnetic coupling. The work demonstrates the control of spin orientation and metamagnetic transitions in layered antiferromagnets, which may provide new perspectives for exploring 2D magnetism and related spintronic devices.

High Pressure‐Driven Magnetic Disorder and Structural Transformation in Fe3GeTe2: Emergence of a Magnetic Quantum Critical Point

“…[ 36–38 ] Our study not only helps resolve the discrepancy noticed above in the pressure‐induced structural change in Fe 3 GeTe 2 , [ 36–38 ] but provides new insights into the underlying mechanism of strain‐mediated magnetism in other vdW magnetic systems. [ 48–51 ] Our study also suggests that Fe 3 GeTe 2 is a perspective candidate material in the search for a pressure‐induced ferromagnetic quantum critical point.…”

Highly Anisotropic Mechanical Response of the Van der Waals Magnet CrPS4

“…[ 17 ] or Peng et al. [ 32 ] ‐ to a negative one ‐ compression of the b‐axis while cooling from room temperature down to 80 K. This structural anisotropy enhancement around 120 K is to our knowledge unreported in literature. This increased anisotropy and expansion of the quasi‐1D chains along the b‐axis upon cooldown illustrates the interplay between lattice parameters and magnetic order that, based on the change in slope of the f 0 ( T ) curve, indicates that magnetic ordering also has a substantial influence on the lattice parameters, leading to further chain expansion.…”

Magnetic van der Waals materials: Synthesis, structure, magnetism, and their potential applications

“…7(b)). [96,234] In-plane anisotropic behaviors of optical properties in CrPS 4 have also been observed. [235][236][237] There is a hidden spin reorientation transition T SR at around 35 K in CrPS 4 with magnetic moments realigning to the b-axis upon heating (Fig.…”