We describe a mechanism by which both a ferroelectric polarization and a magnetization can be created in nonpolar, nonmagnetic materials. Using a combination of phenomenological modeling and first-principles calculations, we demonstrate that ferroelectric polarization, magnetization, or both simultaneously can be transiently induced by an ultrashort laser pulse upon linearly, circularly, or elliptically polarized excitation of phonon modes in $\gamma \text{−}{\text{LiBO}}_2$. The direction and magnitude of the multiferroic polarization can be controlled by the chirality of the laser pulse and the phonon modes, offering a pathway for controlling multiferroicity and magnetoelectricity on ultrafast timescales.

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• Optical phonons
• Ultrafast magnetization dynamics
• Ferroelectrics
• Multiferroics
• Density functional theory