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In bilayer CrI3, experimental and theoretical studies suggest that themagnetic order is closely related to the layer staking configuration. In thiswork, we study the effect of dynamical lattice distortions, induced bynon-linear phonon coupling, in the magnetic order of the bilayer system. We usedensity functional theory to determine the phonon properties and group theoryto obtain the allowed phonon-phonon interactions. We find that the bilayerstructure possesses low-frequency Raman modes that can be non-linearlyactivated upon the coherent photo-excitation of a suitable infrared phononmode. This transient lattice modification, in turn, inverts the sign of theinterlayer spin interaction for parameters accessible in experiments,indicating a low-frequency light-induced antiferromagnet-to-ferromagnettransition.

Phonon-mediated dimensional crossover in bilayer CrI3