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arXiv:2001.07300 · Physical Review Letters

Three-Magnon Bound State in the Quasi-One-Dimensional Antiferromagnet α - NaMnO 2

Rebecca L. Dally, Alvin J. R. Heng, Anna Keselman, Mitchell M. Bordelon, M. B. Stone, Leon Balents, Stephen D. Wilson

Published May 14, 2020• 19 citations
arXivHTMLPDF

Abstract

Here we report on the formation of a three-magnon bound state in the quasi-one-dimensional antiferromagnet α-NaMnO_{2}, where the single-ion, uniaxial anisotropy inherent to the Mn^{3+} ions in this material provides a binding mechanism capable of stabilizing higher order magnon bound states. While such states have long remained elusive in studies of antiferromagnetic chains, neutron scattering data presented here demonstrate that higher order n>2 composite magnons exist, and, specifically, that a weak three-magnon bound state is detected below the antiferromagnetic ordering transition of NaMnO_{2}. We corroborate our findings with exact numerical simulations of a one-dimensional Heisenberg chain with easy-axis anisotropy using matrix-product state techniques, finding a good quantitative agreement with the experiment. These results establish α-NaMnO_{2} as a unique platform for exploring the dynamics of composite magnon states inherent to a classical antiferromagnetic spin chain with Ising-like single ion anisotropy.

DOI
10.1103/physrevlett.124.197203

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Here we report on the formation of a three-magnon bound state in the quasi-one-dimensional antiferromagnet α-NaMnO_{2}, where the single-ion, uniaxial anisotropy inherent to the Mn^{3+} ions in this material provides a binding mechanism capable of stabilizing higher order magnon bound states. While such states have long remained elusive in studies of antiferromagnetic chains, neutron scattering data presented here demonstrate that higher order n>2 composite magnons exist, and, specifically, that a weak three-magnon bound state is detected below the antiferromagnetic ordering transition of NaMnO_{2}. We corroborate our findings with exact numerical simulations of a one-dimensional Heisenberg chain with easy-axis anisotropy using matrix-product state techniques, finding a good quantitative agreement with the experiment. These results establish α-NaMnO_{2} as a unique platform for exploring the dynamics of composite magnon states inherent to a classical antiferromagnetic spin chain with Ising-like single ion anisotropy.
Quasi-one-dimensional materials serve as both testbeds for tractable magnetic models and as a perennial source of intriguing physics. An excellent example is the emergence of multimagnon bound states in ferromagnetic (FM) spin chains, which provide a platform for probing a few-body quantum phenomenon. Despite being studied for many years, the exchange anisotropy-driven bound state of a FM chain has yet to be observed by inelastic neutron scattering (INS). As INS provides a unique window into the nature of magnon-magnon interactions, this represents a substantive gap in the literature. Here, the authors rectify this gap by presenting detailed INS data on the SSS=\textonehalf{} spin chain Li2{}_{2}2​CuO2{}_{2}2​. Their data allows for determination of a refined spin Hamiltonian which fully describes the one-magnon dispersion. With these details in hand, they demonstrate the existence of two-magnon and, potentially, three-magnon bound states in Li2{}_{2}2​CuO2{}_{2}2​, with the potential three-magnon bound state showing anomalous behavior.
We discuss electron spin resonance (ESR) shifts in spin-1 Heisenberg antiferromagnetic chains with a weak single-ion anisotropy, based on several effective field theories: the O(3) nonlinear sigma model (NLSM) in the Haldane phase, free-fermion theories around the lower and the upper critical fields. In the O(3) NLSM, the single-ion anisotropy corresponds to a composite operator which creates two magnons at the same time and position. Therefore, even inside a parameter range where free magnon approximation is valid for thermodynamics, we have to take interactions among magnons into account in order to include the single-ion anisotropy as a perturbation. Although the O(3) NLSM is only valid in the Haldane phase, an appropriate translation of Faddeev-Zamolodchikov operators of the O(3) NLSM to fermion operators enables one to treat ESR shifts near the lower critical field in a similar manner to discussions in the Haldane phase. Our theory gives quantitative agreements with a numerical evaluation using quantum Monte Carlo simulation, and also with recent ESR experimental results on a spin-1 chain compound Ni(C5H14N2)2N3(PF6)\mathrm{Ni}{({\mathrm{C}}_{5}{\mathrm{H}}_{14}{\mathrm{N}}_{2})}_{2}{\mathrm{N}}_{3}({\mathrm{PF}}_{6})Ni(C5​H14​N2​)2​N3​(PF6​).
Few-magnon bound states in quantum spin chains have been long studied and attracted much recent attention. For a higher-spin ferromagnetic XXZ chain with single-ion anisotropy, several features regarding the evolution of the low-lying two-magnon bound states with varying wave number were observed in the literature. However, most of these observations are only qualitatively understood due to the lack of analytical tools. By combining a set of exact two-magnon Bloch states and a plane-wave ansatz, we achieve a complete solution of the two-magnon problem in such a system. We identify parameter regions that support different types of two-magnon bound states, with the boundaries defined by algebraic equations. We discover a narrow region in which two single-ion bound states coexist. We show that the phase diagrams for distinct wave numbers are similar to each other, which enables us to map the evolution of the bound states to the rectilinear movement of a representative point for given parameters in a rescaled phase diagram. This dynamic picture provides quantitative interpretations of the observed features.
We study few-magnon excitations in a finite-size spin-SSS chain with ferromagnetic nearest-neighbor (NN) interaction J>0J>0J>0 and antiferromagnetic next-nearest-neighbor (NNN) interaction ${J}^{\ensuremath{'}}<0$, in the presence of the single-ion (SI) anisotropy DDD. We first reveal the condition for the emergence of zero-excitation-energy states. In the isotropic case with $\mathrm{\ensuremath{\Delta}}={\mathrm{\ensuremath{\Delta}}}^{\ensuremath{'}}=1$ ($\mathrm{\ensuremath{\Delta}}$ and ${\mathrm{\ensuremath{\Delta}}}^{\ensuremath{'}}$ are the corresponding anisotropy parameters), a threshold of $J/|{J}^{\ensuremath{'}}|$, above which the ground state is ferromagnetic, is determined by exact diagonalization for short chains up to 12 sites. Using a set of exact two-magnon Bloch states, we then map the two-magnon problem to a single-particle one on an effective open chain with both NN and NNN hoppings. The whole two-magnon excitation spectrum is calculated for large systems, and the commensurate-incommensurate transition in the lowest-lying mode is found to exhibit different behaviors between S=1/2S=1/2S=1/2 and higher spins due to the interplay of the SI anisotropy and the NNN interaction. For the commensurate momentum $k=\ensuremath{-}\ensuremath{\pi}$, the effective lattice is decoupled into two NN open chains that can be exactly solved via a plane-wave ansatz. Based on this, we analytically identify in the ${\mathrm{\ensuremath{\Delta}}}^{\ensuremath{'}}\ensuremath{-}D/|{J}^{\ensuremath{'}}|$ plane the regions supporting the SI or NNN exchange two-magnon bound states near the edge of the band. In particular, we prove that there always exists a lower-lying NN exchange two-magnon bound state near the band edge for arbitrary $S\ensuremath{\ge}1/2$. Finally, we numerically calculate the nnn-magnon spectra for S=1/2S=1/2S=1/2 with $n\ensuremath{\le}5$ by using a spin-operator matrix element method. The corresponding nnn-magnon commensurate instability regions are determined for finite chains, and consistent results with prior literature are observed.
A full description of a series of spin-wave measurements in CsNiCl3{\mathrm{CsNiCl}}_{3}CsNiCl3​ in the three-dimensional (3D) and one-dimensional (1D) phases and their analysis to provide the first experimental evidence for the Haldane gap is presented. Neutron scattering experiments were performed on a single crystal of CsNiCl3{\mathrm{CsNiCl}}_{3}CsNiCl3​ with both (h,0,l) and (h,h,l) as the scattering plane. The order parameter in both 3D phases was measured and the spin-wave dispersion determined in the lower phase. The spin-wave spectrum calculated from a dynamic susceptibility method was compared with the experimental response in the lower 3D phase to obtain the following values for the exchange and anisotropy constants: J=0.345\ifmmode\pm\else\textpm\fi{}0.008 THz, J'=0.0060\ifmmode\pm\else\textpm\fi{}0.005 THz, and D=-0.0130\ifmmode\pm\else\textpm\fi{}0.0015 THz. These parameters confirm that CsNiCl3{\mathrm{CsNiCl}}_{3}CsNiCl3​ in its disordered phase is a good approximation to a one-dimensional Heisenberg antiferromagnet. In the 1D phase the gap frequency for an isolated chain of Ni2+{\mathrm{Ni}}^{2+}Ni2+ ions is found to be 0.32 THz close to the gap estimated in finite-chain calculations. The results constitute experimental support for the Haldane conjecture that the excitations of integer-spin chains, unlike half-integer--spin chains, exhibit an apparent anisotropy that arises not from the underlying isotropic Hamiltonian, but from many-body effects.