In bilayer $\mathrm{Cr}{\mathrm{I}}_3$, experimental and theoretical studies suggest that the magnetic order is closely related to the layer staking configuration. In this work, we study the effect of dynamical lattice distortions, induced by nonlinear phonon coupling, in the magnetic order of the bilayer system. We use density functional theory to determine the phonon properties and group theory to obtain the allowed phonon-phonon interactions. We find that the bilayer structure possesses low-frequency Raman modes that can be nonlinearly activated upon the coherent photoexcitation of a suitable infrared phonon mode. This transient lattice modification in turn inverts the sign of the interlayer spin interaction for parameters accessible in experiments, indicating a low-frequency light-induced antiferromagnet-to-ferromagnet transition.

• Received 30 March 2020
• Accepted 7 August 2020

DOI:https://doi.org/10.1103/PhysRevB.102.081117