Coherent helicity-dependent spin-phonon oscillations in the ferromagnetic van der Waals crystal CrI3

Padmanabhan, P.; Buessen, F. L.; Tutchton, R.; Kwock, K. W. C.; Gilinsky, S.; Lee, M. C.; McGuire, M. A.; Singamaneni, S. R.; Yarotski, D. A.; Paramekanti, A.; Zhu, J. -X.; Prasankumar, R. P.

doi:10.1038/s41467-022-31786-3

Coherent helicity-dependent spin-phonon oscillations in the ferromagnetic van der Waals crystal CrI3

Journal Article · Tue Aug 02 00:00:00 EDT 2022 · Nature Communications

DOI:https://doi.org/10.1038/s41467-022-31786-3· OSTI ID:1879558

; ; Tutchton, R.; ; ; Lee, M. C.; ; Singamaneni, S. R.; Yarotski, D. A.; Paramekanti, A.; ;

Abstract

The discovery of two-dimensional systems hosting intrinsic magnetic order represents a seminal addition to the rich landscape of van der Waals materials. CrI ₃ 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 CrI ₃ 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 CrI ₃ and highlight its potential for applications requiring high-speed control of magnetism at the nanoscale.

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Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: National Science Foundation; National Science Foundation (NSF); Natural Sciences and Engineering Research Council (NSERC) of Canada; Natural Sciences and Engineering Research Council (NSERC), Canada; USDOE; USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: 89233218CNA000001; AC02-05CH11231; AC05-00OR22725; NA0003960

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 Journal Issue: 1 Vol. 13; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

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