Exotic Magnetic and Electronic Properties of Layered CrI3 Single Crystals Under High Pressure

Abstract

Through advanced experimental techniques on CrI${}_3$ single crystals, we derive a previously not discussed pressure-temperature phase diagram. We find that $T_c$ increases to $\sim$ 66\,K with pressure up to $\sim$ 3\,GPa followed by a decrease to $\sim$ 10\,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 U on Cr 3$d$ orbitals. The origin of the pressure induced reduction of the ordering temperature is associated with a decrease of the calculated bond angle, from 95${}^{\circ }$ at ambient pressure to $\sim$ 85${}^{\circ }$ at 25\,GPa. Above 22\,GPa, the magnetically ordered state is essentially quenched, possibly driving the system to a Kitaev spin-liquid state at low temperature, thereby opening up the possibility of further exploration of long-range quantum entanglement between spins. The pressure-induced semiconductor-to-metal phase transition was revealed by high-pressure resistivity that is accompanied by a transition from a robust ferromagnetic state to gradually more dominating anti-ferromagnetic interactions and was consistent with theoretical modeling.

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• Uniaxial pressure effects in the two-dimensional van-der-Waals ferromagnet CrI${}_3$
• Strong uniaxial pressure dependencies evidencing spin-lattice coupling and spin fluctuations in Cr${}_2$Ge${}_2$Te${}_6$
• Superexchange and spin-orbit coupling in monolayer and bilayer chromium trihalides
• Spin-orbit coupling controlled two-dimensional magnetism in chromium trihalides