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arXiv:2604.06700

Magnon harmonic generation in antiferromagnets: Dynamical symmetry enriched by symmetry breaking

Yuto Jita, Minoru Kanega, Takumi Ogawa, Shunsuke C. Furuya, Masahiro Sato

cond-mat.str-elcond-mat.mes-hallcond-mat.stat-mechquant-phSubmitted Apr 8, 2026• Announced Apr 9, 2026
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Abstract

In recent years, techniques of intense THz laser have enabled us to experimentally observe nonlinear spin dynamics in antiferromagnets since the elementary excitations such as magnons reside on a THz to GHz range in antiferromagnets and THz laser thus can directly excite them. We numerically and theoretically investigate THz-laser or GHz-wave driven harmonic generations in typical ordered phases of antiferromagnets: Néel, canted and weak ferromagnetic phases. The radiation waves (harmonic generations) are created by the incident-wave driven magnon dynamics. We point out that magnetic orders and phase transitions can change the spectra of harmonic generations, differently from those of metallic, semiconductor, or atomic-gas systems without (spontaneous) symmetry breakings. We consider both the magnon harmonic generation driven by standard single-color laser and that by two-color laser in the antiferromagnets, and find several dynamical symmetries and the corresponding selection rules of the harmonic generations. These results indicate that the magnon harmonic generation spectra provide new information about symmetry or symmetry breaking of antiferromagnets.

Comments
38 pages (2 column version), 17 figures

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•Nov 10, 2013•0 citations
In recent years, techniques of intense THz laser have enabled us to experimentally observe nonlinear spin dynamics in antiferromagnets since the elementary excitations such as magnons reside on a THz to GHz range in antiferromagnets and THz laser thus can directly excite them. We numerically and theoretically investigate THz-laser or GHz-wave driven harmonic generations in typical ordered phases of antiferromagnets: Néel, canted and weak ferromagnetic phases. The radiation waves (harmonic generations) are created by the incident-wave driven magnon dynamics. We point out that magnetic orders and phase transitions can change the spectra of harmonic generations, differently from those of metallic, semiconductor, or atomic-gas systems without (spontaneous) symmetry breakings. We consider both the magnon harmonic generation driven by standard single-color laser and that by two-color laser in the antiferromagnets, and find several dynamical symmetries and the corresponding selection rules of the harmonic generations. These results indicate that the magnon harmonic generation spectra provide new information about symmetry or symmetry breaking of antiferromagnets.
In frustrated magnets, a variety of novel phenomena arise due to their peculiar magnetic states, whose excitations usually reside in the GHz to THz range. Intense THz lasers, therefore, lead to examining nonlinear optical effects in such magnets. Employing an unbiased numerical method, we calculate the laser-pulse driven harmonic spectra of the Shastry-Sutherland magnets, which are well known as the model of a quantum frustrated magnet SrCu2\mathrm{SrCu}{}_{2}SrCu2​(BO3\mathrm{BO}{}_{3}BO3​)2{}_{2}2​. As a result, nonlinear responses of triplons and a two-triplon bound state are numerically shown to emerge through the Zeeman or magnetoelectric couplings between the laser and the electron spin. Furthermore, the dynamical symmetries and selection rules of harmonic spectra for the Shastry-Sutherland model realized in SrCu2\mathrm{SrCu}{}_{2}SrCu2​(BO3\mathrm{BO}{}_{3}BO3​)2{}_{2}2​, are derived. The selection rules tell us that one can obtain information on magnetic anisotropy and symmetry from the spectra by manipulating external fields or two-color lasers. Our results indicate that laser-driven harmonic spectra are useful as a probe of less-detectable quantum many-body states in frustrated magnets.
We theoretically study THz-light-driven high-harmonic generation (HHG) in the spin-liquid states of the Kitaev honeycomb model with a magnetostriction coupling between spin and electric polarization.To compute the HHG spectra, we numerically solve the Lindblad equation, taking account of the dissipation effect.We find that isotropic Kitaev models possess a dynamical symmetry, which is broken by a static electric field, analogous to HHG in electron systems.We show that the HHG spectra exhibit characteristic continua of Majorana fermion excitations, and their broad peaks can be controlled by applying static electric or magnetic fields.In particular, the magnetic-field dependence of the HHG spectra drastically differs from those of usual ordered magnets.These results indicate that an intense THz laser provides a powerful tool to observe dynamic features of quantum spin liquids.
This work combines theory and experiment to examine the mechanisms underlying the harmonic generation of magnons. We develop a nonlinear spin-wave framework that is directly analogous to harmonic generation in nonlinear optics, and combine it with scanning nitrogen-vacancy (NV) center magnetometry to image and quantify magnonic harmonic generation in a Ni81_{81}81​Fe19_{19}19​/Pt microstripe. Within this framework, the harmonic response arises from nonlinear magnetization dynamics localized at strongly inhomogeneous textures, such as the sample edges and domain walls, that act as anharmonic confining potentials. Scanning probe imaging confirms that the harmonic response is correspondingly nonuniform and concentrated near the sample edges. We measure an expected nonlinear power-law scaling, a systematic shift toward larger wavevector excitations at higher harmonic order, and a spin-selective response indicative of an increasingly chiral harmonic stray field. These results provide a microscopic understanding of magnonic harmonic generation and highlight its potential for engineering nonlinear functionality in magnonic systems.
In this thesis the elementary excitations of the spin-1=2 Heisenberg antiferromagnet on the square lattice are studied. This fundamental model is a paradigmatic example for long range ordered quantum phases and the spontaneous breaking of a continuous symmetry in condensed matter. The elementary excitations at long wavelengths are well understood by quantized spin waves, i.e., magnons, which are the gapless Goldstone bosons of the broken SU(2) symmetry. However, recent findings reveal an anomalous energy dip at short wavelengths, which cannot be explained by the conventional spin wave theory. The nature of spin waves at short wavelengths remains unclear to this day. A central aim of this thesis is the derivation of an effective magnon description for the square lattice antiferromagnet which is quantitatively valid for all length scales. For this purpose, the method of continuous unitary transformations (CUT) is extended to its use for gapless excitations. CUT methods provide a powerful tool for the derivation of effective quasi-particle descriptions by means of flow equations. However, typical approaches are truncated in real space restricting their scope of application to gapped quantum phases. In order to circumvent these limitations a CUT approach in momentum space is developed. The scaling dimension of operator terms is established as a suitable truncation criterion for gapless quasi-particles. Moreover, a diagrammatic representation of operator terms is introduced which simplifies the derivation and interpretation of flow equations in momentum space. The developed approach is used to transform the Heisenberg Hamiltonian into an effective Hamiltonian which conserves the number of magnons. In addition, effective observables required for the theoretical description of inelastic neutron scattering are derived. The initial magnon operators before the transformation are defined by the Dyson-Maleev representation which leads to a superficially non-hermitian Hamiltonian. As a result, the transformation constitutes a continuous similarity transformation (CST). This formalism enables the formulation of spin wave interactions by means of quartic boson operators. A crucial step of the transformation is the proper renormalization of the spin wave interaction which is achieved by a selfsimilar CST for scaling dimension d = 2. The resulting effective magnon description is consistent at all length scales. In particular, the magnon dispersion exhibits an energy dip at short wavelengths which is in quantitative agreement with recent numerical and experimental data. Further analysis of the spectral properties indicates a strong attraction between spin waves giving rise to a resonance in the longitudinal two-magnon channel. This resonance can be interpreted as the amplitude or Higgs mode of the continuously broken SU(2) symmetry with finite lifetime. The origin of the anomalous dispersion is ascribed to a scattering between the Higgs resonance and single magnon states. The theoretical results are directly compared with experimental data obtained by inelastic neutron scattering and various numerical results which support this view. The quantitative agreement between the effective spin wave approach and numerous numerical and experimental findings shows that magnons are a valid description of the elementary excitations at all length scales. Therefore, this thesis provides a final settlement of the question about the nature of the elementary excitations in the square lattice quantum antiferromagnet.
Currently there is a growing interest in studying the coherent interaction between magnetic systems and electromagnetic radiation in a cavity, prompted partly by possible applications in hybrid quantum systems. We propose a multimode cavity optomagnonic system based on antiferromagnetic insulators, where optical photons couple coherently to the two homogeneous magnon modes of the antiferromagnet. These have frequencies typically in the THz range, a regime so far mostly unexplored in the realm of coherent interactions, and which makes antiferromagnets attractive for quantum transduction from THz to optical frequencies. We derive the theoretical model for the coupled system, and show that it presents unique characteristics. In particular, if the antiferromagnet presents hard-axis magnetic anisotropy, the optomagnonic coupling can be tuned by a magnetic field applied along the easy axis. This allows us to bring a selected magnon mode into and out of a dark mode, providing an alternative for a quantum memory protocol. The dynamical features of the driven system present unusual behavior due to optically induced magnon-magnon interactions, including regions of magnon heating for a red-detuned driving laser. The multimode character of the system is evident in a substructure of the optomagnonically induced transparency window.
We investigate the quantum dynamics of the spins on different Heisenberg antiferromagnetic spin lattice systems. Firstly, we applied the coupled-cluster method to the spin-1/2 antiferromagnetic \emph{XXZ} model on a square lattice by employing an approximation which contains two-body long-range correlations and high-order four-body local correlations. Improvement is found for the ground-state energy, sublattice magnetization, and the critical anisotropy when comparing with the approximation including the two-body correlations alone. We also obtain the full excitation spectrum which is in good agreement with the quantum Monte Carlo results and the high-order spin-wave theory.Secondly, we study the longitudinal excitations of quantum antiferromagnets on a triangular lattice by a recently proposed microscopic many-body approach based on magnon-density waves. We calculate the full longitudinal excitation spectra of the antiferromagnetic Heisenberg model for a general spin quantum number in the isotropic limit. Similar to the square lattice model, we find that, at the center of the first hexagonal Brillouin zone Γ(q=0)\Gamma(\mathbf q=0)Γ(q=0) and at the magnetic ordering wavevectors ±[Q=(4π/3,0)]\pm[\mathbf Q= (4\pi/3,0)]±[Q=(4π/3,0)], the excitation spectra become gapless in the thermodynamic limit, due to the slow, logarithmic divergence of the structure factor. However, these longitudinal modes on two-dimensional models may be considered as quasi-gapped, as any finite-size effect or small anisotropy will induce a large energy gap, when compared with the counterpart of the transverse spin-wave excitations. We have also investigated the excited states of the quasi-one-dimensional quantum antiferromagnets on hexagonal lattices, including the longitudinal modes based on the magnon-density waves. A model Hamiltonian with a uniaxial single-ion anisotropy is first studied by a spin-wave theory based on the one-boson method; the ground state thus obtained is employed for the study of the longitudinal modes. The full energy spectra of both the transverse modes (i.e., magnons) and the longitudinal modes are obtained as functions of the nearest-neighbor coupling and the anisotropy constants. We have found two longitudinal modes due to the non-collinear nature of the triangular antiferromagnetic order, similar to that of the phenomenological field theory approach by Affleck. The excitation energy gaps due to the anisotropy and the energy gaps of the longitudinal modes without anisotropy are then investigated. We then compares our results for the longitudinal energy gaps at the magnetic wavevectors with the experimental results for several antiferromagnetic compounds with both integer and non-integer spin quantum numbers, and we find good agreements after the higher-order contributions are included in our calculations.