Thermal disorder driven magnetic phases in van der Waals magnet CrI3

Magnetic phase transitions often occur spontaneously at specific critical temperatures. The presence of more than one critical temperature (Tc) has been observed in several compounds where the coexistence of competing magnetic orders highlights the importance of phase separation driven by different factors such as pressure, temperature and chemical composition. However, it is unknown whether recently discovered two-dimensional (2D) van der Walls (vdW) magnetic materials show such intriguing phenomena that can result in rich phase diagrams with novel magnetic features to be explored. Here we show the existence of three magnetic phase transitions at different Tc's in 2D vdW magnet CrI3 revealed by a complementary suite of muon spin relaxation-rotation, superconducting quantum interference device magnetometry, and large-scale atomistic simulations including higher-order exchange interactions. We find that the traditionally identified Curie temperature of bulk CrI3 at 61 K does not correspond to the long-range order in the full volume (VM) of the crystal but rather a partial transition with less than 25% of VM being magnetically spin-ordered. This transition is composed of highly disordered domains with the easy-axis component of the magnetization Sz not being fully spin-polarized but disordered by in-plane components (Sx, Sy) over the entire layer. As the system cools down, two additional phase transitions at 50 K and 25 K drive the system to 80% and nearly 100% of the magnetically ordered volume, respectively, where the ferromagnetic ground state has a marked Sz character yet also displaying finite contributions of Sx and Sy to the total magnetization. Our results indicate that volume-wise competing electronic phases play an important role in the magnetic properties of CrI3 which set a much lower threshold temperature for exploitation in magnetic device-platforms than initially considered.