Field-Induced Magnon Decay, Magnon Shadows, and Rotonlike Excitations in the Honeycomb Antiferromagnet YbBr 3
J. A. Hernández, Alexander A. Eberharter, Michael Schuler, Jakob Lass, D. G. Mazzone, Romain Sibille, S. Raymond, Karl W. Krämer, Bruce Normand, B. Roessli, Andreas Martin Läuchli, M. Kenzelmann
Although the search for quantum many-body phenomena in magnetic materials has a strong focus on highly frustrated systems, even unfrustrated quantum magnets show a multitude of unconventional phenomena in their spin excitation spectra. YbBr_{3} is an excellent realization of the S=1/2 antiferromagnetic Heisenberg model on the honeycomb lattice, and we have performed detailed spectroscopic experiments with both unpolarized and polarized neutrons at all applied magnetic fields up to saturation. We observe extensive excitation continua, which cause strong renormalization and the decay of single magnons at higher fields, while coherent features include field-induced "shadows" of the single magnons and the spectacular emergence of a rotonlike excitation. To guide and interpret our experiments, we performed systematic calculations by the method of cylinder matrix-product states that provide quantitative agreement with the neutron scattering data and a qualitative benchmark for the spectral signatures of strong quantum fluctuations even in the absence of magnetic frustration.
Although the search for quantum many-body phenomena in magnetic materials has a strong focus on highly frustrated systems, even unfrustrated quantum magnets show a multitude of unconventional phenomena in their spin excitation spectra. YbBr_{3} is an excellent realization of the S=1/2 antiferromagnetic Heisenberg model on the honeycomb lattice, and we have performed detailed spectroscopic experiments with both unpolarized and polarized neutrons at all applied magnetic fields up to saturation. We observe extensive excitation continua, which cause strong renormalization and the decay of single magnons at higher fields, while coherent features include field-induced "shadows" of the single magnons and the spectacular emergence of a rotonlike excitation. To guide and interpret our experiments, we performed systematic calculations by the method of cylinder matrix-product states that provide quantitative agreement with the neutron scattering data and a qualitative benchmark for the spectral signatures of strong quantum fluctuations even in the absence of magnetic frustration.
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.
Fifty years after Anderson’s resonating valence-bond proposal, the spin-1/2 triangular-lattice Heisenberg antiferromagnet (TLHAF) remains the ultimate platform to explore highly entangled quantum spin states in proximity to magnetic order. Yb-based delafossites are ideal candidate TLHAF materials, which allow experimental access to the full range of applied in-plane magnetic fields. We perform a systematic neutron scattering study of CsYbSe2, first proving the Heisenberg character of the interactions and quantifying the second-neighbor coupling. We then measure the complex evolution of the excitation spectrum, finding extensive continuum features near the 120°-ordered state, throughout the 1/3-magnetization plateau and beyond this up to saturation. We perform cylinder matrix-product-state (MPS) calculations to obtain an unbiased numerical benchmark for the TLHAF and spectacular agreement with the experimental spectra. The measured and calculated longitudinal spectral functions reflect the role of multi-magnon bound and scattering states. These results provide valuable insight into unconventional field-induced spin excitations in frustrated quantum materials.
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 Fifty years after Anderson’s resonating valence-bond proposal, the spin-1/2 triangular-lattice Heisenberg antiferromagnet (TLHAF) remains the ultimate platform to explore highly entangled quantum spin states in proximity to magnetic order. Yb-based delafossites are ideal candidate TLHAF materials, which allow experimental access to the full range of applied in-plane magnetic fields. We perform a systematic neutron scattering study of CsYbSe 2 , first proving the Heisenberg character of the interactions and quantifying the second-neighbor coupling. We then measure the complex evolution of the excitation spectrum, finding extensive continuum features near the 120°-ordered state, throughout the 1/3-magnetization plateau and beyond this up to saturation. We perform cylinder matrix-product-state (MPS) calculations to obtain an unbiased numerical benchmark for the TLHAF and spectacular agreement with the experimental spectra. The measured and calculated longitudinal spectral functions reflect the role of multi-magnon bound and scattering states. These results provide valuable insight into unconventional field-induced spin excitations in frustrated quantum materials.
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.
Field-Induced Spin Excitations in the Spin-1/2 Triangular-Lattice Antiferromagnet CsYbSe2
A layered triangular lattice with spin-1/2 ions is an ideal platform to explore highly entangled exotic states like quantum spin liquid (QSL). Here, we report a systematic in-field neutron scattering study on a perfect two-dimensional triangular-lattice antiferromagnet, CsYbSe2, a member of the large QSL candidate family rare-earth chalcogenides. The elastic neutron scattering measured down to 70 mK shows that there is a short-range 120∘ magnetic order at zero field. In the field-induced ordered states, the spin-spin correlation lengths along the c axis are relatively short, although the heat capacity results indicate long-range magnetic orders at 3 T − 5 T. The inelastic neutron scattering spectra evolve from highly damped continuum-like excitations at zero field to relatively sharp spin wave modes at the plateau phase. Our extensive large-cluster density-matrix renormalization group calculations with a Heisenberg triangular-lattice nearest-neighbor antiferromagnetic model reproduce the essential features of the experimental spectra, including continuum-like excitations at zero field, series of sharp magnons at the plateau phase as well as two-magnon excitations at high energy. This work presents comprehensive experimental and theoretical overview of the unconventional field-induced spin dynamics in triangular-lattice Heisenberg antiferromagnet and thus provides valuable insight into quantum many-body phenomena.