Two-dimensional magnetic materials have emerged as a frontier in condensed matter physics, offering a versatile platform for investigating unprecedented quantum phenomena under extreme conditions. This work focuses on $\mathrm{Mn}\mathrm{P}{\mathrm{S}}_3$, a prototypical Heisenberg antiferromagnet with a Néel temperature ($T_{\mathrm{N}}$) of around 78 K. By combining high-pressure Raman spectroscopy and density functional theory (DFT) calculations, we systematically investigate its phononic and magnetic evolution under compression. Our results reveal a significant pressure-induced enhancement of $T_{\mathrm{N}}$, which rises to 240 K at 20.2 GPa, indicating a substantial strengthening of magnetic coupling. This enhancement is also consistent with the notable blueshift of a possible two-magnon-related magnetic Raman feature. DFT results show that this magnetic evolution is intrinsically linked to a pressure-induced layer-sliding transition occurring near 5 GPa, which triggers a magnetic reconfiguration from interlayer ferromagnetic to interlayer antiferromagnetic coupling. These insights underscore the profound impact of pressure on the structural and magnetic properties of $\mathrm{Mn}\mathrm{P}{\mathrm{S}}_3$, providing critical insights into 2D magnetic systems under extreme conditions and opening new avenues for manipulating the emergent phenomena in low-dimensional magnetic materials via precise pressure control.

Close

PrevNext

View figure in article

• High-pressure studies
• Magnetic coupling
• Magnetic order
• Structural phase transition
• Raman spectroscopy