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Through advanced experimental techniques on CrI$_{3}$ single crystals, wederive a previously not discussed pressure-temperature phase diagram. We findthat $T_{c}$ increases to $\sim$ 66\,K with pressure up to $\sim$ 3\,GPafollowed by a decrease to $\sim$ 10\,K at 21.2\,GPa. The experimental resultsare reproduced by theoretical calculations based on density functional theorywhere electron-electron interactions are treated by a static on-site Hubbard Uon Cr 3$d$ orbitals. The origin of the pressure induced reduction of theordering temperature is associated with a decrease of the calculated bondangle, from 95$^{\circ}$ at ambient pressure to $\sim$ 85$^{\circ}$ at 25\,GPa.Above 22\,GPa, the magnetically ordered state is essentially quenched, possiblydriving the system to a Kitaev spin-liquid state at low temperature, therebyopening up the possibility of further exploration of long-range quantumentanglement between spins. The pressure-induced semiconductor-to-metal phasetransition was revealed by high-pressure resistivity that is accompanied by atransition from a robust ferromagnetic state to gradually more dominatinganti-ferromagnetic interactions and was consistent with theoretical modeling.

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