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.
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Coherent helicity-dependent spin-phonon oscillations in the ferromagnetic van der Waals crystal CrI3
Abstract -
Taylor, A. E. ; Morrow, R. ; Lumsden, M. D. ; Calder, S. ; Upton, M. H. ; Kolesnikov, A. I. ; Stone, M. B. ; Fishman, R. S. ; Paramekanti, A. ; Woodward, P. M. ; et al ( , Physical Review B)
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Hickey, C. ; Rath, P. ; Paramekanti, A. ( , Physical Review B)
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Yuan, Bo ; Clancy, J. P. ; Cook, A. M. ; Thompson, C. M. ; Greedan, J. ; Cao, G. ; Jeon, B. C. ; Noh, T. W. ; Upton, M. H. ; Casa, D. ; et al ( , Physical Review B)
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Ganesh, R. ; Sheng, D. N. ; Kim, Young-June ; Paramekanti, A. ( , Physical Review B)