Field-induced quasi-bound state within the two-magnon continuum of a square-lattice Heisenberg antiferromagnet
Martin Må̊nsson, Frank Elson, Mithilesh Nayak, Alexander A. Eberharter, M. Skoulatos, Simon Ward, U. Stuhr, Niels Bech Christensen, David J. Voneshen, C. Fiolka, Karl Krämer, Christian Rüegg, Henrik Moodysson Rønnow, Bruce Normand, Martin Mourigal, Frédéric Mila, Andreas Martin Läuchli
Abstract Quantum magnets in two dimensions display strong quantum interaction effects even when magnetically ordered. Using the metal-organic framework material CuF 2 (D 2 O) 2 (pyz), we investigate the field-dependent spin dynamics of the S = 1/2 square-lattice Heisenberg antiferromagnet by high-resolution inelastic neutron scattering to applied fields beyond one third of saturation. We discover an anomalously sharp, dispersive “shadow mode” residing within the two-magnon continuum, which shadows the dispersion of the transverse one-magnon branches across the Brillouin zone at an offset equal to the Larmor energy. We perform cylinder matrix-product-state (MPS) calculations that reproduce the field-induced spectrum quantitatively and apply a spectrally consistent 1/ S spin-wave theory to deduce that the “Larmor-shadow mode” is a composite two-magnon resonance: a dispersing magnon at wavevector Q couples to the uniform Larmor precession at Γ, its small intrinsic linewidth indicating a non-perturbative effect of attractive magnon-magnon interactions. Another quantum-fluctuation phenomenon, the zero-field (π, 0) anomaly, is lost at increasing fields, which tighten the spectral weight into the one-magnon and Larmor-shadow modes. To our knowledge, these results constitute the first observation of a sharp quasi-bound state embedded in the continuum of a gapless two-dimensional antiferromagnet.
Abstract Quantum magnets in two dimensions display strong quantum interaction effects even when magnetically ordered. Using the metal-organic framework material CuF 2 (D 2 O) 2 (pyz), we investigate the field-dependent spin dynamics of the S = 1/2 square-lattice Heisenberg antiferromagnet by high-resolution inelastic neutron scattering to applied fields beyond one third of saturation. We discover an anomalously sharp, dispersive “shadow mode” residing within the two-magnon continuum, which shadows the dispersion of the transverse one-magnon branches across the Brillouin zone at an offset equal to the Larmor energy. We perform cylinder matrix-product-state (MPS) calculations that reproduce the field-induced spectrum quantitatively and apply a spectrally consistent 1/ S spin-wave theory to deduce that the “Larmor-shadow mode” is a composite two-magnon resonance: a dispersing magnon at wavevector Q couples to the uniform Larmor precession at Γ, its small intrinsic linewidth indicating a non-perturbative effect of attractive magnon-magnon interactions. Another quantum-fluctuation phenomenon, the zero-field (π, 0) anomaly, is lost at increasing fields, which tighten the spectral weight into the one-magnon and Larmor-shadow modes. To our knowledge, these results constitute the first observation of a sharp quasi-bound state embedded in the continuum of a gapless two-dimensional antiferromagnet.
Quantum magnets in two dimensions display strong quantum interaction effects even when magnetically ordered. Using the metal-organic framework material CuF2(D2O)2(pyz), we investigate the field-dependent spin dynamics of the S=1/2 square-lattice Heisenberg antiferromagnet by high-resolution inelastic neutron scattering to applied fields beyond one third of saturation. We discover an anomalously sharp, dispersive ``shadow mode'' residing within the two-magnon continuum, which shadows the dispersion of the transverse one-magnon branches across the Brillouin zone at an offset equal to the Larmor energy. We perform cylinder matrix-product-state (MPS) calculations that reproduce the field-induced spectrum quantitatively and apply a spectrally consistent 1/S spin-wave theory to deduce that the ``Larmor-shadow mode'' is a composite two-magnon resonance: a dispersing magnon at wavevector Q couples to the uniform Larmor precession at Γ, its small intrinsic linewidth indicating a non-perturbative effect of attractive magnon-magnon interactions. Another quantum-fluctuation phenomenon, the zero-field (π,0) anomaly, is lost at increasing fields, which tighten the spectral weight into the one-magnon and Larmor-shadow modes. To our knowledge, these results constitute the first observation of a sharp quasi-bound state embedded in the continuum of a gapless two-dimensional antiferromagnet.
Abstract The notion of a quasiparticle, such as a phonon, a roton or a magnon, is used in modern condensed matter physics to describe an elementary collective excitation. The intrinsic zero-temperature magnon damping in quantum spin systems can be driven by the interaction of the one-magnon states and multi-magnon continuum. However, detailed experimental studies on this quantum many-body effect induced by an applied magnetic field are rare. Here we present a high-resolution neutron scattering study in high fields on an S=1/2 antiferromagnet C9H18N2CuBr4. Compared with the non-interacting linear spin–wave theory, our results demonstrate a variety of phenomena including field-induced renormalization of one-magnon dispersion, spontaneous magnon decay observed via intrinsic linewidth broadening, unusual non-Lorentzian two-peak structure in the excitation spectra and a dramatic shift of spectral weight from one-magnon state to the two-magnon continuum.
Abstract In ordered quantum magnets where interactions between elementary excitations dominate over their kinetic energy, perturbative approaches often fail, making non-perturbative methods essential to capture spectral features such as bound states and the redistribution of weight within excitation continua. Although an increasing number of experiments report anomalous spin excitation continua in such systems, their microscopic interpretation remains an open challenge. Here, we investigate the spin dynamics of the triangular-lattice antiferromagnet in its 1/3-plateau phase using two complementary non-perturbative approaches: exact diagonalization in a truncated Hilbert space for a gas of elementary excitations (THED) and matrix product state (MPS) simulations. Alongside cross-validation between these methods, we benchmark our results against inelastic neutron scattering (INS) data. The THED analysis confirms the presence of two-magnon bound states and identifies the anomalous scattering continuum observed in both MPS and INS as a two-magnon resonance, arising from hybridization between the bound state and the two-magnon continuum. Furthermore, THED reveals bound states overlapping with the continuum, enriching the interpretation of continuum anomalies. More broadly, THED provides a robust framework for investigating anomalous spin excitation continua and bound-state effects in other materials with gapped spectra. Its combination of accuracy and computational efficiency makes it a powerful tool for extracting reliable microscopic models in semiclassical regimes.
We study the field dependence of the antiferromagnetic spin-21 Heisenberg model on the square lattice by means of exact diagonalizations. In the first part, we calculate the spin-wave velocity c, the spin stiffness ${\ensuremath{\rho}}_{s}$, and the magnetic susceptibility ${\ensuremath{\chi}}_{\ensuremath{\perp}}$, and thus determine the microscopic parameters of the low-energy long-wavelength description. In the second part, we present a comprehensive study of dynamical spin-correlation functions for magnetic fields ranging from zero up to saturation. We find that, at low fields, magnons are well defined in the whole Brillouin zone but the dispersion is substantially modified by quantum fluctuations compared to the classical spectrum. At higher fields, decay channels open and magnons become unstable with respect to multimagnon scattering. Our results directly apply to inelastic neutron-scattering experiments.
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.
In ordered quantum magnets where interactions between elementary excitations dominate over their kinetic energy, perturbative approaches often fail, making non-perturbative methods essential to capture spectral features such as bound states and the redistribution of weight within excitation continua. Although an increasing number of experiments report anomalous spin excitation continua in such systems, their microscopic interpretation remains an open challenge. Here, we investigate the spin dynamics of the triangular-lattice antiferromagnet in its 1/3-plateau phase using two complementary non-perturbative approaches: exact diagonalization in a truncated Hilbert space for a gas of elementary excitations (THED) and matrix product state (MPS) simulations. Alongside cross-validation between these methods, we benchmark our results against inelastic neutron scattering (INS) data. The THED analysis confirms the presence of two-magnon bound states and identifies the anomalous scattering continuum observed in both MPS and INS as a two-magnon resonance, arising from hybridization between the bound state and the two-magnon continuum. Furthermore, THED reveals bound states overlapping with the continuum, enriching the interpretation of continuum anomalies. More broadly, THED provides a robust framework for investigating anomalous spin excitation continua and bound-state effects in other materials with gapped spectra. Its combination of accuracy and computational efficiency makes it a powerful tool for extracting reliable microscopic models in semiclassical regimes.