Van der Waals (vdWs) crystals have attracted a great deal of scientific attention due to their interesting physical properties and widespread practical applications. Among all, CrSiTe3 (CST) is a ferromagnetic semiconductor with the Curie temperature (TC) of ~32 K. In this letter, we study the magnetic properties of bulk CST single-crystal upon proton irradiation with the fluence of 1x1018 protons/cm2. Most significantly, we observed an enhancement (23%) in the saturation magnetization from 3.9 {mu}B to 4.8 {mu}B and is accompanied by an increase in the coercive field (465-542 Oe) upon proton irradiation. Temperature-dependent X-band electron paramagnetic resonance measurements show no additional magnetically active defects/vacancies that are generated upon proton irradiation. The findings from X-ray photoelectron spectroscopy and Raman measurements lead us to believe that modification in the spin-lattice coupling and introduction of disorder could cause enhancement in saturation magnetization. This work demonstrates that proton irradiation is a feasible method in modifying the magnetic properties of vdWs crystals, which represents a significant step forward in designing future spintronic and magneto-electronic applications.
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