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Abstract The discovery of two-dimensional systems hosting intrinsic magnetic order represents a seminal addition to the rich landscape of van der Waals materials. CrI₃is an archetypal example, where the interdependence of structure and magnetism, along with strong light-matter interactions, provides a new platform to explore the optical control of magnetic and vibrational degrees of freedom at the nanoscale. However, the nature of magneto-structural coupling on its intrinsic ultrafast timescale remains a crucial open question. Here, we probe magnetic and vibrational dynamics in bulk CrI₃using ultrafast optical spectroscopy, revealing spin-flip scattering-driven demagnetization and strong transient exchange-mediated interactions between lattice vibrations and spin oscillations. The latter yields a coherent spin-coupled phonon mode that is highly sensitive to the driving pulse’s helicity in the magnetically ordered phase. Our results elucidate the nature of ultrafast spin-lattice coupling in CrI₃and highlight its potential for applications requiring high-speed control of magnetism at the nanoscale. 

Developing functional, cleavable two-dimensional materials for use in next generation devices has recently become a topic of considerable interest due to their unique properties. Of particular interest, transition metal halides CrI3 and CrCl3 have shown to be good contenders for tunable and cleavable magnetic materials due to their unique magnetic properties in the monolayer.