Coherent helicity-dependent spin-phonon oscillations in the ferromagnetic van der Waals crystal CrI3
The discovery of two-dimensional systems hosting intrinsic magnetic order represents a seminal addition to the rich landscape of van der Waals materials. CrI3 is 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 CrI3 using 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 CrI3 and highlight its potential for applications requiring high-speed control of magnetism at the nanoscale.
- Research Organization:
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Sponsoring Organization:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; USDOE Laboratory Directed Research and Development (LDRD) Program; National Science Foundation (NSF); Natural Sciences and Engineering Research Council of Canada (NSERC); USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); Natural Sciences and Engineering Research Council (NSERC), Canada; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
- Grant/Contract Number:
- 89233218CNA000001; 2105109; NA0003960; DMR-1747426; AC02-05CH11231; AC05-00OR22725; NSF-DMR 2105109
- OSTI ID:
- 1879558
- Alternate ID(s):
- OSTI ID: 1884754; OSTI ID: 1975381
- Report Number(s):
- LA-UR-20-27954; 4473; PII: 31786
- Journal Information:
- Nature Communications, Journal Name: Nature Communications Vol. 13 Journal Issue: 1; ISSN 2041-1723
- Publisher:
- Nature Publishing GroupCopyright Statement
- Country of Publication:
- United Kingdom
- Language:
- English
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