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Magnetic van der Waals materials provide an ideal playground for exploringthe fundamentals of low-dimensional magnetism and open new opportunities forultrathin spin processing devices. The Mermin-Wagner theorem dictates that asin reduced dimensions isotropic spin interactions cannot retain long-rangecorrelations; the order is stabilized by magnetic anisotropy. Here, usingultrashort pulses of light, we demonstrate all-optical control of magneticanisotropy in the two-dimensional van der Waals antiferromagnet NiPS$_3$.Tuning the photon energy in resonance with an orbital transition betweencrystal-field split levels of the nickel ions, we demonstrate the selectiveactivation of a sub-THz two-dimensional magnon mode. The pump polarizationcontrol of the magnon amplitude confirms that the activation is governed by theinstantaneous magnetic anisotropy axis emergent in response to photoexcitationof orbital states with a lowered symmetry. Our results establish pumping oforbital resonances as a universal route for manipulating magnetic order inlow-dimensional (anti)ferromagnets.

Controlling the anisotropy of a van der Waals antiferromagnet with light