Direct Magnetic Evidence, Functionalization, and Low-Temperature Magneto-Electron Transport in Liquid-Phase Exfoliated FePS₃

Magnetism and the existence of magnetic order in a material is determined by its dimensionality. In this regard, the recent emergence of magnetic layered van der Waals (vdW) materials provides a wide playground to explore the exotic magnetism arising in the two-dimensional (2D) limit. The magnetism of 2D flakes, especially antiferromagnetic ones, however, cannot be easily probed by conventional magnetometry techniques, being often replaced by indirect methods like Raman spectroscopy. Here, we make use of an alternative approach to provide direct magnetic evidence of few-layer vdW materials, including antiferromagnets. We take advantage of a surfactant-free, liquid-phase exfoliation (LPE) method to obtain thousands of few-layer FePS₃ flakes that can be quenched in a solvent and measured in a conventional SQUID magnetometer. We show a direct magnetic evidence of the antiferromagnetic transition in FePS₃ few-layer flakes, concomitant with a clear reduction of the Néel temperature with the flake thickness, in contrast with previous Raman reports. The quality of the LPE FePS₃ flakes allows the study of electron transport down to cryogenic temperatures. The significant through-flake conductance is sensitive to the antiferromagnetic order transition. Besides, an additional rich spectra of electron transport excitations, including secondary magnetic transitions and potentially magnon-phonon hybrid states, appear at low temperatures. Finally, we show that the LPE is additionally a good starting point for the mass covalent functionalization of 2D magnetic materials with functional molecules. This technique is extensible to any vdW magnetic family.