Pressure-induced transitions in FePS3: Structural, magnetic and electronic properties

FePS3 is a prototype van der Waals layered antiferromagnet and a Mott insulator under ambient conditions, which has been recently reported to go through a pressure-induced dimensionality crossover and an insulator-to-metal transition. These transitions also lead to the appearance of a novel magnetic metallic state. To further understand these emergent structural and physical properties, we have performed a first-principles study using van der Waals and Hubbard U corrected density functional theory including a random structure search. Our computational study attempts to interpret the experimental coexistence of the low- and intermediate-pressure phases and we predict a novel highpressure phase with distinctive dimensionality and different possible origins of metallicity.