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Magnetic insulators in reduced dimension are the ideal model systems to studyspin-crossover(SCO) induced cooperative behavior under pressure. Similar to theexternal perturbations like light illumination or temperature, externalpressure may provide new pathway to accelerate giant lattice collapse,andsubsequently Mott transition in van der Waals (vdW) materials with diminishingeffect of the third dimension. Here, we investigate room-temperaturelayer-dependent SCO and insulator-metal transition in vdW magnet,FePS3, underhigh pressure using micro-Raman scattering.Experimentally obtained spectra, inagreement with the computed Raman modes, indicates evidence of IMT of FePS3started off with a spin-state transition from a high (S=2) to low spin state(S=0) with a thickness dependent critical pressure (P_c) which reduces to 1.45GPa in 3-layer flakes compared to 10.8 GPa for the bulk counterpart.Additionally, a broad Raman mode (P*) emerges between 310 cm^{-1} and 370cm^{-1} at elevated pressure for three different thicknesses of FePS3 flakes(3-100 layers), also corroborated with computational results which suggests thepressure dependent decrease of metal-ligand bond distance(Fe-S) with loweringof magnetic moment in FePS3. Phenomenologically, our results in few-layerflakes with strong structural anisotropy which enhances the in-plane strainwith applied pressure can be understood by adopting Hubbard model andconsidering the spectral-range (bandwidth W) as a function of layer numbers andpressure with a power-law scaling. Reduction of the critical pressure for phasetransition in few-layer vdW magnets to 1-2 GPa marks the possibility of usingnano-enclosure fit for use in device electronics where the pressure is induceddue to interfacial adhesion, like in vdW heterostructure or molecules trappedbetween layers,and thereby,avoiding the conventional use of diamond anvil cell.

Spin-crossover assisted metallization of few-layer FePS$_3$ at 1.45 GPa