Metal phosphorous trichalcogenide is an important group of layered two-dimensional (2D) materials with potentially diverse applications in low-dimensional magnetic and spintronic devices. Herein we present a comprehensive investigation on the lattice dynamics and spin–phonon interactions of mechanically exfoliated atomically thin 2D magnetic material—iron phosphorus trisulfide (FePS ₃ ) by Raman spectroscopy and first principle calculations. Layer-number and temperature dependent Raman spectroscopy suggests a magnetic persistence in FePS ₃ even down to monolayer regime through the spin–phonon coupling, while the Néel temperature decreases from 117 K in bulk to 104 K in monolayer sample. Our studies advocate the intriguing magnetic properties in 2D crystals and suggest that FePS ₃ is a promising candidate material for future magnetic applications.

Magnetic two-dimensional materials have attracted considerable attention for their significant potential application in spintronics. In this study, we present a high-quality Fe-doped SnS₂ monolayer exfoliated using a micromechanical cleavage method. Fe atoms were doped at the Sn atom sites, and the Fe contents are ∼2.1%, 1.5%, and 1.1%. The field-effect transistors based on the Fe_0.021Sn_0.979S₂ monolayer show n-type behavior and exhibit high optoelectronic performance. Magnetic measurements show that pure SnS₂ is diamagnetic, whereas Fe_0.021Sn_0.979S₂ exhibits ferromagnetic behavior with a perpendicular anisotropy at 2 K and a Curie temperature of ~31 K. Density functional theory calculations show that long-range ferromagnetic ordering in the Fe-doped SnS₂ monolayer is energetically stable, and the estimated Curie temperature agrees well with the results of our experiment. The results suggest that Fe-doped SnS₂ has significant potential in future nanoelectronic, magnetic, and optoelectronic applications.