Exotic Magnetic and Electronic Properties of Layered Formula Presented Single Crystals under High Pressure

Abstract

Through advanced experimental techniques on Formula Presented single crystals, we derive a pressure-temperature phase diagram. We find that Formula Presented increases to Formula Presented K with pressure up to Formula Presented GPa followed by a decrease to Formula Presented K at 21.2 GPa. The experimental results are reproduced by theoretical calculations based on density functional theory where electron-electron interactions are treated by a static on-site Hubbard Formula Presented on Cr Formula Presented orbitals. The origin of the pressure-induced reduction of the ordering temperature is associated with a decrease in the calculated bond angle, from Formula Presented at ambient pressure to Formula Presented at 25 GPa. Above 22 GPa, experiment and theory jointly point to the idea that the ferromagnetically ordered state is destroyed, giving rise first to a complex, unknown magnetic configuration, and at sufficiently high pressures a pure antiferromagnetic configuration. This sequence of transitions in the magnetism is accompanied by a well-detected pressure-induced semiconductor-to-metal phase transition that is revealed by both high-pressure resistivity measurements and ab initio theory. ©2022 American Physical Society.