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Ultrafast and coherent generation of magnons is of great significance forhigh-speed antiferromagnetic spintronics. One possible route is byexciton-magnon pairwise optical excitation. To date, such exciton-magnontransitions have been studied mostly by linear optical means in a limitednumber of conventional three-dimensional antiferromagnets. Here we investigatethis correlated transition in van der Waals antiferromagnet MnPS$_3$ by usingresonant second-harmonic generation spectroscopy, a nonlinear optical probesensitive to the symmetry of electronic and magnetic excitations. Twoexciton-magnon peaks are observed, in line with the exciton-induced splittingof magnon density of states predicted by a Koster-Slater type theory,indicating significant exciton-magnon interactions. In addition, a large linearmagnetoelectric effect of excitons is observed. These findings provide renewedunderstandings on the correlation effects in two-dimensional magnets withenhanced quasiparticle scattering cross-sections, and point to potentialcoherent control among charge, spin and orbital degrees of freedom intwo-dimensional magnets by optical means.

Exciton-magnon splitting in van der Waals antiferromagnet MnPS$_3$ unveiled by second-harmonic generation