Pressure-Dependent Magnetic Properties of Quasi-2D Cr₂Si₂Te₆ and Mn₃Si₂Te₆

Recently, pressure has been used to induce structuraland magneticphase transitions in many layered quantum materials whose layers arelinked by van der Waals forces. Materials with such weakly held layersallow for relatively easy manipulation of the superexchange mechanism,which can give rise to novel magnetic behavior. Using hydrostaticpressure as a disorderless means to manipulate the interlayer coupling,we applied pressure on two quasi-2D sister compounds, namely, Cr2Si2Te6 (CST) and Mn3Si2Te6 (MST), up to similar to 1 GPa. Magnetic propertymeasurements with the application of pressure revealed that the ferromagnetictransition temperature decreases in CST, while the opposite occursfor the ferrimagnetic MST. In MST, magnetization decreases with theincrease in pressure, and such a trend is not clearly observed withinthe pressure range studied for CST. The overall pressure effect onmagnetic characteristics such as exchange couplings and magnetic anisotropyenergies is also examined theoretically using density functional theory.Exchange coupling in MST is strongly frustrated, and the first nearestneighbor interaction is the most dominant of the components with thestrongest pressure dependence. In CST, the exchange coupling parametersexhibit very little dependence on pressure. This combined experimentaland theoretical work has the potential to expand to other relevantquantum materials.