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Ultrafast control of magnetic interactions via light-driven phonons

Abstract

Resonant ultrafast excitation of infrared-active phonons is a powerful technique with which to control the electronic properties of materials that leads to remarkable phenomena such as the light-induced enhancement of superconductivity1,2, switching of ferroelectric polarization3,4 and ultrafast insulator-to-metal transitions5. Here, we show that light-driven phonons can be utilized to coherently manipulate macroscopic magnetic states. Intense mid-infrared electric field pulses tuned to resonance with a phonon mode of the archetypical antiferromagnet DyFeO3 induce ultrafast and long-living changes of the fundamental exchange interaction between rare-earth orbitals and transition metal spins. Non-thermal lattice control of the magnetic exchange, which defines the stability of the macroscopic magnetic state, allows us to perform picosecond coherent switching between competing antiferromagnetic and weakly ferromagnetic spin orders. Our discovery emphasizes the potential of resonant phonon excitation for the manipulation of ferroic order on ultrafast timescales6.

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Fig. 1: Phonon-driven reconfiguration of the magnetic potential in DyFeO3.
Fig. 2: Ultrafast dynamics of the soft mode frequency.
Fig. 3: Out-of-equilibrium metastable magnetic state.
Fig. 4: Ultrafast phonon-induced magnetic phase transition.

Data availability

All data presented in this work are publicly available with identifier https://doi.org/10.5281/zenodo.4338556. Source data are provided with this paper.

Code availability

The TB2J code for calculating the exchange interactions is freely available under the BSD 2 clause license and can be found at https://github.com/mailhexu/TB2J/. The Abinit code for the DFT calculations is an open source code with GNU General Public License and is freely available at https://www.abinit.org/.

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Acknowledgements

We thank S. Heirman for assistance in measuring the linear absorption in the MIR spectral range, E. Lesne for the X-ray diffraction measurements and E. Demler, R. Citro, M. Cuoco and T. C. van Thiel for fruitful discussions. This work was supported by the EU through the European Research Council, grant no. 677458 (AlterMateria), the Netherlands Organization for Scientific Research (NWO/OCW) as part of the Frontiers of Nanoscience programme (NanoFront) and the VENI-VIDI-VICI programme, the European Union’s Seventh Framework Programme (FP7/2007–2013)/ERC grant agreement no. 339813 (Exchange), ERC Grant agreement 852050 (MAGSHAKE), the programme Leading Scientist of the Russian Ministry of Science and Higher Education (14.Z50.31.0034), the Ministry of Science and Higher Education of the Russian Federation in the framework of Increase Competitiveness Program of NUST MISiS (grant no. K2-2019-006), implemented by a governmental decree dated 16 March 2013, N211. E.B. and A.S. thank the FRS-FNRS, ARC AIMED project, the CÉCI supercomputer facilities (grant no. 2.5020.1) and Tier-1 supercomputer of the Fédération Wallonie-Bruxelles funded by the Walloon Region (grant no. 1117545).

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A.D.C. conceived the project together with D.A. D.A. and J.R.H. carried out the experiments and analysed the data. R.V.M. and A.V.K. identified the material system for the project and contributed to the analysis. B.A.I. and Y.M.B. contributed to the theoretical treatment of the experimental results. A.S. and E.B. performed the DFT calculations. All the authors discussed the results. The manuscript was written by D.A., J.R.H. and A.D.C. with feedback from all the co-authors.

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Correspondence to D. Afanasiev or A. D. Caviglia.

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Afanasiev, D., Hortensius, J.R., Ivanov, B.A. et al. Ultrafast control of magnetic interactions via light-driven phonons. Nat. Mater. 20, 607–611 (2021). https://doi.org/10.1038/s41563-021-00922-7

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