Abstract
Identifying efficient pathways to control and modify the order parameter of a macroscopic phase in materials is an important ongoing challenge. One way to do this is via the excitation of a high-frequency mode that couples to the order, and this is the ultimate goal of the field of ultrafast phase transitions1,2. This is an especially interesting research direction in magnetism, where the coupling between spin and lattice excitations is required for magnetization reversal3,4. However, previous attempts5,6 have not demonstrated switching between magnetic states via resonant pumping of phonon modes. Here we show how an ultrafast resonant excitation of the longitudinal optical phonon modes in magnetic garnet films switches magnetization into a peculiar quadrupolar magnetic domain pattern, revealing the magneto-elastic mechanism of the switching. In contrast, the excitation of strongly absorbing transverse phonon modes results in a thermal demagnetization effect only.
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Data availability
All other data that support the plots within this paper and other findings of this study are available from the corresponding author on reasonable request. Source data are provided with this paper.
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Acknowledgements
We acknowledge support from the Foundation for Polish Science uner grant number POIR.04.04.00-00-413C/17, as well as from the COST Action grant number CA17123 MAGNETOFON. We acknowledge the Nederlandse Organisatie voor Wetenschappelijk Onderzoek (NWO-I) for their financial contribution, including the support of the FELIX Laboratory. We thank A. Maziewski for discussions as well as T. Rasing for continuous support. We acknowledge Y.-L. Mathis for support at the IR1 beamline of the Karlsruhe Research Accelerator (KARA).
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A.S. and A.K. conceived the project. A.S. performed the magneto-optical imaging together with C.S.D. D.A., K.S. and A.C. performed time-resolved magnetization dynamics measurements. K.S.R. and A.V.B. performed IR ellipsometry measurements. C.S.D. performed the micromagnetic simulations. A.S., A.K., A.V.B. and A.V.K. jointly discussed the result and wrote the manuscript.
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Peer review information Nature Physics thanks Zhao-Hua Cheng and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.
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Extended data
Extended Data Fig. 1 Magnetization states in YIG.
Magnetic domains pattern with four magnetization states in relation to the crystal symmetry in YIG/GGG(001). The large stripe-like domains are formed that have magnetizations along the [1–11] and the [11–1] axes. Within them, small domains are found that possess magnetization along the [111] and the [1-1-1] axes. Magnetization orientations in the domains and type of the domain structure have been identified following the procedure explained in refs. 18,36.
Extended Data Fig. 2 Profiles of magnetic domains.
Top panel from left to right shows the images of domain structures before the laser excitation (a), after irradiation at pump wavelength 14 μm (b) and difference of these images (c). The laser spot was marked by red dashed circle. The initial domain structure was observed by applying an external in-plane magnetic field 10 mT along the [1-10] axis for one second. The graph shows the spatial profiles of the intensity from the difference image with magnetic contrast after irradiation. The profiles of intensity in the azimuthal directions ϕ1, ϕ2 and ϕ3 are marked on image (c). Тhe red solid line represents the beam profile (half part) of irradiation pulse. The images are 210 × 210 μm2 large.
Extended Data Fig. 3 Phonon spectra of YIG.
Complex dielectric function ε(ω) = ε1(ω) + iε2(ω) (black) and the imaginary part of the dielectric loss functions Im(−1/ε) (red) of YIG obtained by direct inversion of ellipsometric spectra. Vertical dashed lines indicate zero crossing of ε1(ω).
Extended Data Fig. 4 Phonon spectra of GGG.
Imaginary parts of the dielectric function ε(ω) (black) and the loss function -1/ε(ω) (blue) for Gd3Ga5O12. The shaded background shows the infrared transmission spectrum of 7.3 μm thick YIG:Co. The 15% to 20% transparency region around the LO mode at 490 cm−1 is marked by the dotted lines in Extended Data Figs. 3 and 5.
Extended Data Fig. 5 Infrared absorption and loss function.
Absorption coefficient (black) and imaginary part of the loss function (red) of YIG determined from ellipsometric spectra.
Extended Data Fig. 6 Domain structures after demagnetization.
The images of magnetic domain structures before the laser excitation (a), after irradiation at pump wavelength 17 μm with fluence 1.2 J·cm−2. (b) and the image of sample damage after irradiation with fluence 2.5 J·cm−2. The difference images between before and after irradiation with fluence 0.3 J·cm−2 (d), 0.7 J·cm−2 (e) 1.2 J·cm−2 (f). The laser spot was marked by red dashed circle. The white arrows are marked the crystallographic axes in the YIG film.
Extended Data Fig. 7 Ultrafast magnetization precession in YIG.
Time-resolved magnetization precession induced by the femtosecond pump pulses in YIG film. The out-of-plane component of the magnetization is detected with the help of time-resolved magneto-optical Faraday rotation. (a) The magnetization precession measured using different pump wavelengths in the range from 8 μm to 17 μm. (b) Dependence of the normalized precession amplitude on the pump wavelength (black points) and magnetization switching (blue points) from Fig. 2. The normalized precession amplitude is calculated as the ratio of the precession amplitude to the maximal amplitude obtained for 14 um pump laser-induced with pump fluence 0.06 J·cm−2. The red solid lines are fits of damped harmonic oscillations. The frequency of the precession for different pump wavelengths is constantly 4.54 ± 0.25 GHz.
Extended Data Fig. 8 Spatial distribution of magneto-elastic energy.
Magneto-elastic energy distribution created by the excitation of the phonon mode: (a) symmetric part with b2 = 0 (the arrows on the axes indicate x−y coordinates), and (b) antisymmetric part with b1 = 0.
Extended Data Fig. 9 Simulation of magnetization switching for different anisotropy parameters.
Micromagnetic simulations of switching after the application of the strain pulse with different anisotropy environments. All material parameters are the same as those described in the Methods, except for the following modifications. (a) The easy axes of the cubic magnetocrystalline anisotropy are aligned along [100], [010] and [001]. (b) An additional uniaxial magnetic anisotropy (strength Ku = −0.25 kJ·m−3) is inserted with its easy axis aligned along [100]. (c) Same as in (b) except the strain pulse amplitude is reduced by 20%. The arrows and the color-coding indicate the orientation of the magnetization in the x−y plane after the application of the single strain pulse with duration 1 ps.
Supplementary information
Supplementary Video 1
Time-resolved magnetization switching. The video shows the results of micromagnetic calculations, performed using the same parameters as discussed in the Methods. The top panel shows the time-resolved amplitude of the strain field. Two strain pulses of strength 5.7 T and full-width at half-duration 1 ps are used, separated in time by 20 ps. The bottom panel shows the time-resolved spatial distribution of magnetization. Both the colour coding and the arrows (the latter are subsampled by 10) indicate the orientation of magnetization in the x–y plane.
Source data
Source Data Fig. 2
Statistical source data.
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Stupakiewicz, A., Davies, C.S., Szerenos, K. et al. Ultrafast phononic switching of magnetization. Nat. Phys. 17, 489–492 (2021). https://doi.org/10.1038/s41567-020-01124-9
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DOI: https://doi.org/10.1038/s41567-020-01124-9
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