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Terahertz-field-driven magnon upconversion in an antiferromagnet

Nature Physics (2024)Cite this article

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Abstract

Excitation and nonlinear control of lattice vibrations with light has become a powerful method to manipulate the properties of quantum materials out of equilibrium. Generalizing from coherent phonon–phonon interactions to nonlinear couplings among other types of collective mode would open additional opportunities to design the dynamic properties of solids. For example, the collective excitations of magnetic order—magnons—can carry information with little energy dissipation, and their coherent and nonlinear control would provide an attractive route to achieve collective-mode-based information processing and storage in forthcoming spintronics and magnonics. Here we discover that intense terahertz fields can initiate the processes of magnon upconversion mediated by an intermediate magnetic resonance. By utilizing two-dimensional terahertz polarimetry, we demonstrate the unidirectional nature of coupling between distinct magnon modes of a canted antiferromagnet. The calculations of spin dynamics further suggest that this coupling is a universal feature of antiferromagnets with canted magnetic moments. These results demonstrate a route to induce desirable energy transfer pathways and a terahertz-induced coupling between coherent magnons in solids.

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Fig. 1: THz-field-driven magnon responses and THz polarimetry on ErFeO3 at room temperature.
Fig. 2: Two-dimensional THz spectroscopy of the magnon upconversion signal at room temperature.
Fig. 3: Temperature dependence of magnon upconversion.
Fig. 4: Origin of the magnon upconversion process.

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Data availability

The data presented in this work are available via Zenodo at https://zenodo.org/records/10050662.

Code availability

The codes used to perform the simulations and analyse the data in this work are available from the corresponding authors upon request.

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Acknowledgements

Z.Z., Z.-J.L., E.R.S. and K.A.N acknowledge support from the US Department of Energy (DOE), Office of Basic Energy Sciences, under award no. DE-SC0019126. Work at UT Austin was primarily supported by the Robert A. Welch Foundation (F-2092-20220331) (to F.Y.G. for data taking and analysis) and the United States Army Research Office (W911NF-23-1-0394) (to E.B. for data interpretation, manuscript writing and supervision). Y.-C.C. acknowledges direct funding from the MIT UROP. S.C. and W.R. acknowledge support from the Science and Technology Commission of Shanghai Municipality (no. 21JC1402600) and the National Natural Science Foundation of China (NSFC; nos. 12074242, 12374116 and 12074241). JC and PN were supported by the Quantum Science Center (QSC), a National Quantum Information Science Research Center of the U.S. Department of Energy (DOE). P.N. acknowledges support as a Moore Inventor Fellow through grant no. GBMF8048 from the Gordon and Betty Moore Foundation and from the John Simon Guggenheim Memorial Foundation (Guggenheim Fellowship). A.v.H. gratefully acknowledges funding by the Humboldt Foundation.

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Author notes

  1. These authors contributed equally: Zhuquan Zhang, Frank Y. Gao.

Authors and Affiliations

  1. Department of Chemistry, Massachusetts Institute of Technology, Cambridge, MA, USA

    Zhuquan Zhang, Yu-Che Chien, Zi-Jie Liu, Eric R. Sung & Keith A. Nelson

  2. Department of Physics, The University of Texas at Austin, Austin, TX, USA

    Frank Y. Gao & Edoardo Baldini

  3. College of Letters and Science, University of California, Los Angeles, CA, USA

    Jonathan B. Curtis & Prineha Narang

  4. Department of Physics, Materials Genome Institute and International Center for Quantum and Molecular Structures, Shanghai University, Shanghai, China

    Xiaoxuan Ma, Wei Ren & Shixun Cao

  5. Department of Physics, Massachusetts Institute of Technology, Cambridge, MA, USA

    Alexander von Hoegen

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Contributions

Z.Z. conceived the study. Z.Z. and F.Y.G. designed and performed the experiments and analysed the data, supported by Z.-J.L. and Y.-C.C. Z.Z., Y.-C.C. and F.Y.G. performed the spin dynamics simulations, supported by J.B.C. and E.R.S. X.M. grew and cut the high-quality single crystals used in the experiments under the guidance of W.R. and S.C. Z.Z., F.Y.G., J.B.C., P.N., A.v.H., E.B. and K.A.N. interpreted the data. Z.Z., F.Y.G., E.B., A.v.H. and K.A.N. led the paper preparation with input from all the authors. K.A.N. and E.B. supervised the project.

Corresponding authors

Correspondence to Shixun Cao, Edoardo Baldini or Keith A. Nelson.

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Zhang, Z., Gao, F.Y., Chien, YC. et al. Terahertz-field-driven magnon upconversion in an antiferromagnet. Nat. Phys. (2024). https://doi.org/10.1038/s41567-023-02350-7

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