The discovery of long-range magnetic ordering in atomically thin materials catapulted the van der Waals (vdW) family of compounds into an unprecedented popularity. In particular, with a current push in space exploration, it is beneficial to study how the properties of such materials evolve under proton irradiation. Owing to their robust intra-layer stability and sensitivity to external perturbations, these materials provide excellent opportunities for studying proton irradiation as a non-destructive tool for controlling their magnetic properties. Specifically, the exfoliable Cr2Si2Te6 (CST) is a ferromagnetic semiconductor with the Curie temperature (TC) of ~32 K. Here, we have investigated the magnetic properties of CST upon proton irradiation as a function of fluence (1 x 1015, 5 x 1015, 1 x 1016, 5 x 1016, and 1 x 1018 H+/cm2) by employing variable-temperature, variable-field magnetization measurements coupled with electron paramagnetic resonance (EPR) spectroscopy and detail how the magnetization, magnetic anisotropy and EPR spectral parameters vary as a function of proton fluence across the magnetic phase transition. While the TC remains constant as a function of proton fluence, we observed that the saturation magnetization and magnetic anisotropy diverge at the proton fluence of 5 x 1016 H+/cm2, which is prominent in the ferromagnetic phase, in particular. This work demonstrates that proton irradiation is a feasible method for modifying the magnetic properties and local magnetic interactions of vdWs crystals, which represents a significant step forward in the design of future spintronic and magneto-electronic applications.
