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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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.
References
Strogatz, S. H. Nonlinear Dynamics and Chaos: With Applications to Physics, Biology, Chemistry, and Engineering (CRC Press, 2018).
Foias, C. et al. Navier-Stokes Equations and Turbulence Vol. 83 (Cambridge Univ. Press, 2001).
Friston, K. J. Book review: brain function, nonlinear coupling, and neuronal transients. Neuroscientist 7, 406–418 (2001).
Först, M. et al. Nonlinear phononics as an ultrafast route to lattice control. Nat. Phys. 7, 854–856 (2011).
Kozina, M. et al. Terahertz-driven phonon upconversion in SrTiO3. Nat. Phys. 15, 387–392 (2019).
Mankowsky, R. et al. Nonlinear lattice dynamics as a basis for enhanced superconductivity in YBa2Cu3O6.5. Nature 516, 71–73 (2014).
Li, X. et al. Terahertz field–induced ferroelectricity in quantum paraelectric SrTiO3. Science 364, 1079–1082 (2019).
Nova, T. et al. Metastable ferroelectricity in optically strained SrTiO3. Science 364, 1075–1079 (2019).
Nova, T. F. et al. An effective magnetic field from optically driven phonons. Nat. Phys. 13, 132–136 (2017).
Disa, A. S. et al. Polarizing an antiferromagnet by optical engineering of the crystal field. Nat. Phys. 16, 937–941 (2020).
Afanasiev, D. et al. Ultrafast control of magnetic interactions via light-driven phonons. Nat. Mater. 20, 607–611 (2021).
Stupakiewicz, A. et al. Ultrafast phononic switching of magnetization. Nat. Phys. 17, 489–492 (2021).
Juraschek, D. M., Wang, D. S. & Narang, P. Sum-frequency excitation of coherent magnons. Phys. Rev. B 103, 094407 (2021).
Hortensius, J. et al. Coherent spin-wave transport in an antiferromagnet. Nat. Phys. 17, 1001–1006 (2021).
Bae, Y. J. et al. Exciton-coupled coherent magnons in a 2D semiconductor. Nature 609, 282–286 (2022).
Chumak, A. V. et al. Magnon spintronics. Nat. Phys. 11, 453–461 (2015).
Michael, M. H. et al. Parametric resonance of Josephson plasma waves: a theory for optically amplified interlayer superconductivity in YBa2Cu3O6+x. Phys. Rev. B 102, 174505 (2020).
Juraschek, D. M., Meier, Q. N. & Narang, P. Parametric excitation of an optically silent Goldstone-like phonon mode. Phys. Rev. Lett. 124, 117401 (2020).
Curtis, J. B. et al. Cavity magnon-polaritons in cuprate parent compounds. Phys. Rev. Research 4, 013101 (2022).
Kiselev, S. I. et al. Microwave oscillations of a nanomagnet driven by a spin-polarized current. Nature 425, 380–383 (2003).
Lu, J. et al. Coherent two-dimensional terahertz magnetic resonance spectroscopy of collective spin waves. Phys. Rev. Lett. 118, 207204 (2017).
Kurihara, T. et al. Observation of terahertz-induced dynamical spin canting in orthoferrite magnon by magnetorefractive probing. Commun. Phys. 6, 51 (2023).
Zhang, Z. et al. Generation of third-harmonic spin oscillation from strong spin precession induced by terahertz magnetic near fields. Nat. Commun. 14, 1795 (2023).
Mukai, Y. et al. Nonlinear magnetization dynamics of antiferromagnetic spin resonance induced by intense terahertz magnetic field. New J. Phys. 18, 013045 (2016).
Schlauderer, S. et al. Temporal and spectral fingerprints of ultrafast all-coherent spin switching. Nature 569, 383–387 (2019).
Baierl, S. et al. Nonlinear spin control by terahertz-driven anisotropy fields. Nat. Photon. 10, 715–718 (2016).
Mashkovich, E. et al. Terahertz optomagnetism: nonlinear THz excitation of GHz spin waves in antiferromagnetic FeBO3. Phys. Rev. Lett. 123, 157202 (2019).
Yamaguchi, K. et al. Terahertz time-domain observation of spin reorientation in orthoferrite ErFeO3 through magnetic free induction decay. Phys. Rev. Lett. 110, 137204 (2013).
Li, X. et al. Observation of Dicke cooperativity in magnetic interactions. Science 361, 794–797 (2018).
Teo, S. M. et al. Single-shot THz detection techniques optimized for multidimensional THz spectroscopy. Rev. Sci. Instrum. 86, 051301 (2015).
Gao, F. Y. et al. High-speed two-dimensional terahertz spectroscopy with echelon-based shot-to-shot balanced detection. Opt. Lett. 47, 3479–3482 (2022).
Grishunin, K. et al. Excitation and detection of terahertz coherent spin waves in antiferromagnetic α-Fe2O3. Phys. Rev. B. 104, 024419 (2021).
Johnson, C. L., Knighton, B. E. & Johnson, J. A. Distinguishing nonlinear terahertz excitation pathways with two-dimensional spectroscopy. Phys. Rev. Lett. 122, 073901 (2019).
Mahmood, F. et al. Observation of a marginal Fermi glass. Nat. Phys. 17, 627–631 (2021).
Mashkovich, E. A. et al. Terahertz light–driven coupling of antiferromagnetic spins to lattice. Science 374, 1608–1611 (2021).
Zhang, Y. et al. Nonlinear rotational spectroscopy reveals many-body interactions in water molecules. Proc. Natl Acad. Sci. USA 118, e2020941118 (2021).
Gorodetsky, G. & Lüthi, B. Sound-wave-soft-mode interaction near displacive phase transitions: spin reorientation in ErFeO3. Phys. Rev. B 2, 3688 (1970).
Khalsa, G., Benedek, N. A. & Moses, J. Ultrafast control of material optical properties via the infrared resonant Raman effect. Phys. Rev. X 11, 021067 (2021).
Brächer, T., Pirro, P. & Hillebrands, B. Parallel pumping for magnon spintronics: amplification and manipulation of magnon spin currents on the micron-scale. Phys. Rep. 699, 1–34 (2017).
Lisenkov, I., Jander, A. & Dhagat, P. Magnetoelastic parametric instabilities of localized spin waves induced by traveling elastic waves. Phys. Rev. B 99, 184433 (2019).
Carmiggelt, J. J. et al. Broadband microwave detection using electron spins in a hybrid diamond-magnet sensor chip. Nat. Commun. 14, 490 (2023).
Yeh, K.-L. et al. Generation of high average power 1 kHz shaped THz pulses via optical rectification. Opt. Commun. 281, 3567–3570 (2008).
Gao, F. Y. et al. Snapshots of a light-induced metastable hidden phase driven by the collapse of charge order. Sci. Adv. 8, eabp9076 (2022).
Noe, G. T. et al. Single-shot terahertz time-domain spectroscopy in pulsed high magnetic fields. Opt. Express 24, 30328–30337 (2016).
Duchi, M. et al. 2D-Raman-THz spectroscopy with single-shot THz detection. J. Chem. Phys. 155, 174201 (2021).
Kampfrath, T. et al. Coherent terahertz control of antiferromagnetic spin waves. Nat. Photon. 5, 31–34 (2011).
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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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.
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Zhang, Z., Gao, F.Y., Chien, YC. et al. Terahertz-field-driven magnon upconversion in an antiferromagnet. Nat. Phys. 20, 788–793 (2024). https://doi.org/10.1038/s41567-023-02350-7
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DOI: https://doi.org/10.1038/s41567-023-02350-7
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