Comparative structural evolution under pressure of powder and single crystals of the layered antiferromagnet <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:msub><mml:mrow><mml:mi>FePS</mml:mi></mml:mrow><mml:mn>3</mml:mn></mml:msub></mml:math>
Abstract
${\mathrm{FePS}}_{3}$ is a layered magnetic van der Waals compound that undergoes a Mott insulator-metal transition under applied pressure. The transition has an associated change in the crystal symmetry and magnetic structure. Understanding the underlying physics of these transitions requires a detailed understanding of the crystal structure as a function of pressure. Two conflicting models have previously been proposed for the evolution of the structure with pressure. To settle the disagreement, we present a study of the pressure-dependent crystal structures using both single-crystal and powder x-ray diffraction measurements. We show unambiguously that the highest-pressure transition involves a collapse of the interplanar spacing, along with an increase in symmetry from a monoclinic to a trigonal space group, to the exclusion of other models. Our collected results are crucial for understanding high-pressure behavior in these materials and demonstrate a clear and complete methodology for exploring complex two-dimensional material structures under pressure.