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arXiv:2006.10922 · Physical Review Letters

Coexistence and Interaction of Spinons and Magnons in an Antiferromagnet with Alternating Antiferromagnetic and Ferromagnetic Quantum Spin Chains

Heda Zhang, Zhiying Zhao, Dominique Gautreau, Marcin Raczkowski, Akash Saha, Vasile Ovidiu Garlea, Huibo B. Cao, Tao Hong, Harald O. Jeschke, S. D. Mahanti, Turan Birol, Fakher F. Assaad, Xianglin Ke

Published Jul 17, 2020• 25 citations
arXivHTMLPDF

Abstract

In conventional quasi-one-dimensional antiferromagnets with quantum spins, magnetic excitations are carried by either magnons or spinons in different energy regimes: they do not coexist independently, nor could they interact with each other. In this Letter, by combining inelastic neutron scattering, quantum Monte Carlo simulations, and random phase approximation calculations, we report the discovery and discuss the physics of the coexistence of magnons and spinons and their interactions in Botallackite-Cu_{2}(OH)_{3}Br. This is a unique quantum antiferromagnet consisting of alternating ferromagnetic and antiferromagnetic spin-1/2 chains with weak interchain couplings. Our study presents a new paradigm where one can study the interaction between two different types of magnetic quasiparticles: magnons and spinons.

DOI
10.1103/physrevlett.125.037204

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In conventional quasi-one-dimensional antiferromagnets with quantum spins, magnetic excitations are carried by either magnons or spinons in different energy regimes: they do not coexist independently, nor could they interact with each other. In this Letter, by combining inelastic neutron scattering, quantum Monte Carlo simulations, and random phase approximation calculations, we report the discovery and discuss the physics of the coexistence of magnons and spinons and their interactions in Botallackite-Cu_{2}(OH)_{3}Br. This is a unique quantum antiferromagnet consisting of alternating ferromagnetic and antiferromagnetic spin-1/2 chains with weak interchain couplings. Our study presents a new paradigm where one can study the interaction between two different types of magnetic quasiparticles: magnons and spinons.
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Many phenomena in magnetism can be described using classical models, yet magnetism is a quantum mechanical effect. In addition to thermal fluctuations, quantum fluctuations arise due to the quantum uncertainty of the ground state. These fluctuations are enhanced by low dimensionality and low spin. Spin chains show interesting excitations associated with quasiparticles. Model materials for spin chains can be realized in compounds where the interchain interactions are weak enough. This thesis presents neutron scattering studies of two model materials for spin chains with different spin symmetry. The spin2 Heisenberg antiferromagnetic chain CuSO4*5D2O has a main exchange of J ∼ 3 K, which permits to study its excitation spectrum up to temperatures of ten times the exchange. The spin2 Heisenberg magnet has been studied widely both theoretically and experimentally. The excitation spectrum of the spin2 Heisenberg antiferromagnet consists of quasiparticles called spinons, and calculations for it exist for T = 0 and as a function of temperature. A quantitative comparison between experimental data and theoretical models across a range of temperatures is presented. The excitation spectrum of CuSO4*5D2O is excellently described by the excitation spectrum of a spin2 Heisenberg antiferromagnetic chain at finite temperatures. Energy-temperature scaling is observed at temperatures up to 2J . For these temperatures the Luttinger liquid description of the spin2 Heisenberg antiferromagnetic chain is valid. A spinon continuum is confirmed at all measured temperatures. Therefore, even at ten times the main exchange (T ≈ 10 J), CuSO4*5D2O shows the behavior of a quantum magnet, and not of a classical system at infinite temperatures, for which one would expect single spin flips. The Ising chain is one of the most studied models in magnetism, one model compound for it is RbCoCl3. Optical spectroscopy measurements suggest a lower gap than for similar compounds, which makes it better suited for high resolution neutron spectroscopy. Magnetic correlations along the chains arise in RbCoCl3 below 80 K. A gapped continuum is observed, which arises from isolated antiferromagnetic Ising chains. Below the first magnetic ordering temperature TN1 ≈ 28 K bound states are observed, which arise due to correlations which form between the chains. Strong diffuse scattering leads to the conclusion that disorder is still present. At the second magnetic ordering transition, at TN2 ≈ 14 K, the bound states split as the correlations between the chains change. Fits indicate that the correlations change continuously as a function of temperature. Above TN2 the excitation spectrum of RbCoCl3 can be described by a spin1 2 Ising chain with an XY-component which is treated as a perturbation. Below TN2 the main features are reproduced correctly, but deviations from the details indicate that additional terms in the Hamiltonian may be necessary. This thesis was carried out at the Institut Laue-Langevin, the Laboratory for Neutron Scattering and Imaging at the Paul Scherrer Institute and ETH Zurich.
Abstract Using quantum Monte Carlo, exact diagonalization, and perturbation theory, we study the spectrum of the S = 1/2 antiferromagnetic Heisenberg trimer chain by varying the ratio g = J2/J1 of the intertrimer and intratrimer coupling strengths. The doublet ground states of trimers form effective interacting S = 1/2 degrees of freedom described by a Heisenberg chain. Therefore, the conventional two-spinon continuum of width ∝ J1 when g = 1 evolves into to a similar continuum of width ∝ J2 when g → 0. The intermediate-energy and high-energy modes are termed doublons and quartons which fractionalize with increasing g to form the conventional spinon continuum. In particular, at g ≈ 0.716, the gap between the low-energy spinon branch and the high-energy band with mixed doublons, quartons, and spinons closes. These features should be observable in inelastic neutron scattering experiments if a quasi-one-dimensional quantum magnet with the linear trimer structure and J2 < J1 can be identified. Our results may open a window for exploring the high-energy fractional excitations.
An S=1∕2S=1∕2S=1∕2 ferromagnetic (F) and antiferromagnetic (AF) random alternating Heisenberg quantum spin chain model is investigated in connection to its realization compound ${(\mathrm{C}{\mathrm{H}}_{3})}_{2}\mathrm{C}\mathrm{H}\mathrm{N}{\mathrm{H}}_{3}\mathrm{Cu}{({\mathrm{Cl}}_{x}{\mathrm{Br}}_{1\ensuremath{-}x})}_{3}$. The exchange interaction bonds consist of alternating strong F-AF random bonds and weak uniform AF bonds. Using the quantum Monte Carlo method we have found that the excitation energy gap closes and the uniform AF order becomes critical in the intermediate-concentration region. This finding explains the experimental observation of the magnetic transition by considering weak interchain interactions. The present results suggest that uniform AF order survives even in the presence of randomly located ferromagnetic bonds. This may be an exotic quantum effect.
Low dimensionality enhances quantum fluctuations, triggering novel states of quantum matter to emerge. In real materials, low dimensionality usually arises from spatially strongly anisotropic couplings. Here, we demonstrate a different mechanism: in two-dimensional systems with coupled alternating ferromagnetic (FM) and antiferromagnetic (AFM) spin-1/21/21/2 chains, an applied magnetic field may drive a dimensional reduction. Under magnetic field, the FM chains polarize and stiffen, suppressing the propagation of transverse AFM fluctuations from one chain to another, and effectively induce one-dimensional behavior at low energies. For a model describing botallackite, Cu2_22​(OH)3_33​Br, quantum Monte Carlo dynamics show that beyond a critical magnetic field, the low-energy spectrum reduces to that of a one-dimensional AFM Heisenberg spin-1/21/21/2 chain with field-dependent incommensurate two-spinon fluctuations, providing clear signatures for inelastic neutron scattering.
Two quasi-one-dimensional S=1S=1S=1 quantum antiferromagnetic materials, PbNi2V2O8{\mathrm{PbNi}}_{2}{\mathrm{V}}_{2}{\mathrm{O}}_{8}PbNi2​V2​O8​ and SrNi2V2O8,{\mathrm{SrNi}}_{2}{\mathrm{V}}_{2}{\mathrm{O}}_{8},SrNi2​V2​O8​, are studied by inelastic neutron scattering on powder samples. A simple model Hamiltonian is proposed for the two systems and used to analyze the data. Quantitative information on in-chain and interchain interactions obtained from this analysis is discussed in the context of qualitatively different ground-state properties: magnetic long-range order in SrNi2V2O8{\mathrm{SrNi}}_{2}{\mathrm{V}}_{2}{\mathrm{O}}_{8}SrNi2​V2​O8​ and disordered ``spin liquid'' Haldane-gap state in PbNi2V2O8.{\mathrm{PbNi}}_{2}{\mathrm{V}}_{2}{\mathrm{O}}_{8}.PbNi2​V2​O8​.