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We study how the color and polarization of ultrashort pulses of visible lightcan be used to control the demagnetization processes of the antiferromagneticinsulator Cr$_2$O$_3$. We utilize time-resolved second harmonic generation(SHG) to probe how changes in the magnetic and structural state evolve in time.We show that, varying the pump photon-energy to excite either localizedtransitions within the Cr or charge transfer states, leads to markedlydifferent dynamics. Through a full polarization analysis of the SHG signal,symmetry considerations and density functional theory calculations, we showthat, in the non-equilibrium state, SHG is sensitive to {\em both} latticedisplacements and changes to the magnetic order, which allows us to concludethat different excited states couple to phonon modes of different symmetries.Furthermore, the spin-scattering rate depends on the induced distortion,enabling us to control the timescale for the demagnetization process. Ourresults suggest that selective photoexcitation of antiferromagnetic insulatorsallows fast and efficient manipulation of their magnetic state.

Resonant optical control of the structural distortions that drive ultrafast demagnetization in Cr$_2$O$_3$