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The discovery of long-range magnetic ordering in atomically thin materialscatapulted the van der Waals (vdW) family of compounds into an unprecedentedpopularity. In particular, with a current push in space exploration, it isbeneficial to study how the properties of such materials evolve under protonirradiation. Owing to their robust intra-layer stability and sensitivity toexternal perturbations, these materials provide excellent opportunities forstudying proton irradiation as a non-destructive tool for controlling theirmagnetic properties. Specifically, the exfoliable Cr2Si2Te6 (CST) is aferromagnetic semiconductor with the Curie temperature (TC) of ~32 K. Here, wehave investigated the magnetic properties of CST upon proton irradiation as afunction of fluence (1 x 1015, 5 x 1015, 1 x 1016, 5 x 1016, and 1 x 1018H+/cm2) by employing variable-temperature, variable-field magnetizationmeasurements coupled with electron paramagnetic resonance (EPR) spectroscopyand detail how the magnetization, magnetic anisotropy and EPR spectralparameters vary as a function of proton fluence across the magnetic phasetransition. While the TC remains constant as a function of proton fluence, weobserved that the saturation magnetization and magnetic anisotropy diverge atthe proton fluence of 5 x 1016 H+/cm2, which is prominent in the ferromagneticphase, in particular. This work demonstrates that proton irradiation is afeasible method for modifying the magnetic properties and local magneticinteractions of vdWs crystals, which represents a significant step forward inthe design of future spintronic and magneto-electronic applications.

Proton-fluence dependent magnetic properties of exfoliable quasi-2D van der Waals Cr2Si2Te6 magnet