Engineering photomagnetism in collinear van der Waals antiferromagnets

Abstract: Achieving efficient ultrafast optical control of antiferromagnetic spin dynamics is a central goal for next-generation high-speed THz spintronic and magnonic devices. Resonant optical pumping of crystal-field-split d-d orbital multiplets in magnetic TM ions directly modulates exchange and spin-orbit interactions, inducing large-amplitude coherent spin precession. However, such effects are limited to a handful of systems and there is no general strategy to enhance d-d photomagnetism in antiferromagnets. Here, we demonstrate the engineering of photomagnetism via TM-ion doping in collinear van der Waals antiferromagnets. In Mn$<em>{1-x}$Ni$_x$PS$_3$, small amounts of Ni$<sup>{2+}$ activate a strong photomagnetic response while largely preserving the Néel ground state. Even 10% Ni boosts the response by more than an order of magnitude compared to pure MnPS$_3$, with resonant pumping of Ni$<sup>{2+}$ d-d transitions driving large-amplitude coherent spin precession and providing helicity-dependent phase control. Tuning the pump energy across the full Mn$</em>{1-x}$Ni$_x$PS$_3$ composition range shows that Ni excitations remain effective across competing Néel and zig-zag antiferromagnetic states while supporting tunable-frequency coherent spin precession. These results establish TM-ion doping as a versatile strategy to harness orbital multiplet excitations for ultrafast, low-dissipation spin control in van der Waals antiferromagnets.