Three-wave mixing of anharmonically coupled magnons

Magnons are quantized collective spin-wave excitations in magnetically ordered systems. Revealing their interactions among these collective modes is crucial for the understanding of fundamental many-body effects in such systems and the development of high-speed information transport and processing devices based on them. Nevertheless, identifying couplings between individual magnon modes remains a long-standing chal-lenge. Here, we observe unambiguous spectroscopic fingerprints of anharmonic coupling between distinct magnon modes in an antiferromagnet, as evidenced by coherent photon emission at the sum and difference frequencies of the two modes. This discovery is enabled by driving two magnon modes coherently with a pair of tailored terahertz fields and then disentangling a mixture of nonlinear responses with different origins, symmetries, and field dependences in a two-dimensional frequency-frequency correla-tion map. Our approach provides a new platform for generating nonlinear magnon-magnon mixings and establishes a systematic means of unveiling intricate couplings among distinct low-energy collective modes.

[1]  K. Nelson,et al.  Nonlinear coupled magnonics: Terahertz field-driven magnon upconversion , 2022 .

[2]  Zhuquan Zhang,et al.  High-speed two-dimensional terahertz spectroscopy with echelon-based shot-to-shot balanced detection. , 2022, Optics letters.

[3]  Michael E. Ziebel,et al.  Exciton-coupled coherent magnons in a 2D semiconductor , 2022, Nature.

[4]  R. Pisarev,et al.  Terahertz light–driven coupling of antiferromagnetic spins to lattice , 2021, Science.

[5]  M. Oshikawa,et al.  Photon Echo from Lensing of Fractional Excitations in Tomonaga-Luttinger Spin Liquid , 2021, Physical Review X.

[6]  G. Ma,et al.  Ultrastrong magnon–magnon coupling dominated by antiresonant interactions , 2020, Nature Communications.

[7]  R. Nandkishore,et al.  Spectroscopic fingerprints of gapped quantum spin liquids, both conventional and fractonic , 2020, Physical Review Research.

[8]  Hao Zhang,et al.  Hybridized quadrupolar excitations in the spin-anisotropic frustrated magnet FeI2 , 2020, 2004.05623.

[9]  A. Cavalleri,et al.  Author Correction: Polarizing an antiferromagnet by optical engineering of the crystal field , 2020, Nature Physics.

[10]  Yong Baek Kim,et al.  Theory of Two-Dimensional Nonlinear Spectroscopy for the Kitaev Spin Liquid. , 2019, Physical review letters.

[11]  T. Nattermann,et al.  Direct evidence of spatial stability of Bose-Einstein condensate of magnons , 2019, Nature Communications.

[12]  Y. Wan,et al.  Resolving Continua of Fractional Excitations by Spinon Echo in THz 2D Coherent Spectroscopy. , 2019, Physical review letters.

[13]  P. Jarillo-Herrero,et al.  Gigahertz Frequency Antiferromagnetic Resonance and Strong Magnon-Magnon Coupling in the Layered Crystal CrCl_{3}. , 2019, Physical review letters.

[14]  Michael J. Hoffmann,et al.  Terahertz-driven phonon upconversion in SrTiO3 , 2018, Nature Physics.

[15]  S. Louie,et al.  Discovery of intrinsic ferromagnetism in two-dimensional van der Waals crystals , 2017, Nature.

[16]  K. Nelson,et al.  Coherent Two-Dimensional Terahertz Magnetic Resonance Spectroscopy of Collective Spin Waves. , 2016, Physical review letters.

[17]  K. Nelson,et al.  Invited Article: Single-shot THz detection techniques optimized for multidimensional THz spectroscopy. , 2015, The Review of scientific instruments.

[18]  M. Bonn,et al.  Single-pulse terahertz coherent control of spin resonance in the canted antiferromagnet YFeO3, mediated by dielectric anisotropy , 2013 .

[19]  A. Cavalleri,et al.  Nonlinear phononics as an ultrafast route to lattice control , 2011, 1101.1878.

[20]  Alfred Leitenstorfer,et al.  Coherent terahertz control of antiferromagnetic spin waves , 2011 .

[21]  Makoto Nakajima,et al.  Coherent control of spin precession motion with impulsive magnetic fields of half-cycle terahertz radiation. , 2010, Physical review letters.

[22]  Daniel B. Turner,et al.  Coherent measurements of high-order electronic correlations in quantum wells , 2010, Nature.

[23]  Daniel B. Turner,et al.  Two-Quantum 2D FT Electronic Spectroscopy of Biexcitons in GaAs Quantum Wells , 2009, Science.

[24]  K. Nelson,et al.  Generation of high average power 1 kHz shaped THz pulses via optical rectification , 2008 .

[25]  A. Serga,et al.  Bose–Einstein condensation of quasi-equilibrium magnons at room temperature under pumping , 2006, Nature.

[26]  M. Wortis Bound States of Two Spin Waves in the Heisenberg Ferromagnet , 1963 .

[27]  T. Moriya Anisotropic Superexchange Interaction and Weak Ferromagnetism , 1960 .

[28]  I. Dzyaloshinsky A thermodynamic theory of “weak” ferromagnetism of antiferromagnetics , 1958 .

[29]  R. Peierls Zur Theorie der Metalle , 1933 .