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

TL;DR

This study explores how high pressure affects the magnetic and electronic properties of layered CrI3 crystals, revealing a phase diagram with increased and then decreased transition temperatures, a pressure-induced metal transition, and potential quantum spin-liquid states.

Contribution

It provides the first detailed pressure-temperature phase diagram of CrI3, combining experimental data with theoretical modeling to uncover pressure-induced magnetic and electronic phase transitions.

Findings

$T_c$ increases to ~66K at 3 GPa, then decreases to ~10K at 21.2 GPa.

Pressure induces a semiconductor-to-metal transition and a shift from ferromagnetic to antiferromagnetic interactions.

Above 22 GPa, magnetism is quenched, possibly leading to a Kitaev spin-liquid state.

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.