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Optical pump-probe experiments carried out in the time domain reveal both theintrinsic low energy dynamics and its connections to higher energy excitationsin correlated electron systems. In this work, we propose two microscopicmechanisms for the optical generation of coherent magnetic modes in van derWaals magnets, and derive the corresponding effective light-spin interactions:either through pumping atomic orbital excitations resonantly or via alight-induced Floquet spin Hamiltonian, the ground state of the system isdriven out of equilibrium. The subsequent long-time relaxational dynamics canthen be probed using, e.g. the magneto-optical Kerr effect or transient gratingspectroscopy. As an example, we apply our framework to NiPS$_3$, which ismagnetically ordered in the bulk, and is conjectured to realize the XY model inthe monolayer limit. Our theory makes explicit how the material's low-energyresponse depends sensitively on the microscopic details of the light-spincoupling as well as pump fluence, frequency and polarization. For the case ofbulk NiPS$_3$, we find quantitative agreement with recent experiments byAfanasiev et al. [Science Advances 7, abf3096 (2021)]. We further proposepump-probe experiments for monolayer NiPS$_3$ and detail how anomalousrelaxational behaviour may reveal excitations of a (proximate) BKT phase in aproposed effective XY model.

Ultrafast optical excitation of magnetic dynamics in van der Waals magnets: Coherent magnons and BKT dynamics in NiPS$_3$