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Recently, the pressure has been used as external stimuli to induce structuraland magnetic phase transitions in many layered quantum materials whose layersare linked by van der Waals forces. Such materials with weakly held layersallow relatively easy manipulation of the superexchange mechanism and lead tonovel magnetic behavior. Using the hydrostatic pressure as a disorderless meansto manipulate the interlayer coupling, we applied pressure on two quasi-2Dsister compounds, namely, Cr2Si2Te6 (CST) and Mn3Si2Te6 (MST), up to ~1 GPa.Magnetic property measurements with the application of pressure revealed thatthe ferromagnetic transition temperature decreases in CST while the oppositetrend occurs for the ferrimagnet MST. In MST, the magnetization decreases withthe increase in the pressure, and such trend is not clearly noticed in CST,within the pressure range studied. Theoretical calculations showed the overallpressure effect on layer separation, bond angle, and exchange coupling,strongly influencing the change in subsequent magnetic characteristics.Exchange coupling in Mn3Si2Te6 is strongly frustrated and the first nearestneighbor interaction is the most dominant of the components with the strongestpressure dependence. Whereas, in Cr2Si2Te6, the exchange coupling parametersexhibit very little dependence on the pressure. This combined experimental andtheoretical work has the potential to expand to other relevant quantummaterials.

Pressure-induced magnetic properties of quasi-2D Cr2Si2Te6 and Mn3Si2Te6