Cu 2 Fe 2 Ge 4 O 13 is a quantum magnet consisting of Cu spin dimers and Fe spin chains. It shows an antiferromagnetic phase transition at low temperatures due to the magnetic moment of Fe. Since the two parts are weakly coupled, magnetic excitations are well separated into high-energy Cu dimer part and low-energy Fe chain part. We study the magnetic excitations in the ordered phase of Cu 2 Fe 2 Ge 4 O 13 based on a theory used for coupled spin dimer systems such as TlCuCl 3 . Analyzing the dynamical spin correlation functions, we find several high-energy modes with longitudinal spin fluctuations peculiar to the coupled spin dimer and spin chain system. This is consistent with the recent experimental result of inelastic neutron scattering. A possibility to detect such longitudinal modes is discussed by means of magnetic Raman scattering.
Cu 2 Fe 2 Ge 4 O 13 is a quantum magnet consisting of Cu spin dimers and Fe spin chains. It shows an antiferromagnetic phase transition at low temperatures due to the magnetic moment of Fe. Since the two parts are weakly coupled, magnetic excitations are well separated into high-energy Cu dimer part and low-energy Fe chain part. We study the magnetic excitations in the ordered phase of Cu 2 Fe 2 Ge 4 O 13 based on a theory used for coupled spin dimer systems such as TlCuCl 3 . Analyzing the dynamical spin correlation functions, we find several high-energy modes with longitudinal spin fluctuations peculiar to the coupled spin dimer and spin chain system. This is consistent with the recent experimental result of inelastic neutron scattering. A possibility to detect such longitudinal modes is discussed by means of magnetic Raman scattering.
Low-dimensional quantum magnets provide an ideal platform to explore spin-lattice coupling-mediated quantum correlations, which give rise to emergent quasiparticle excitations. The antiferromagnetically coupled spin-1/2 trimer chain of copper ions in Na2Cu3Ge4O12 (NCGO) hosts high-energy spin excitations of different species, whose energy scales overlap with those of lattice vibrations. Here, we report a comprehensive temperature-dependent Raman spectroscopic study performed between 80 and 400 K. The dynamic spin susceptibility, as obtained from the analysis of the broad spectral background, reveals the emergence of quasiparticle excitations below 170 K. We further identify an unusual crossover of phonon dynamics when the material transits from a normal paramagnetic state to a correlated quantum magnetic state. A power law dependence of the integrated Raman susceptibility of the phonon modes, Iχ′′i∼∣T−Tc∣β, is observed with the critical temperature Tc=167$\pm$1 K, and critical exponent β=0.24±0.02. The combined results obtained from the broad spectral background and sharp phonon peaks further indicate that the phonon renormalization observed across the crossover is driven by dynamic spin states. Additionally, statistical correlations among phonon energy eigenvalues, quantified through matrix-norm and power-test analyses of 200 spectra recorded at 80 K, reveal an unexpected linear correlation among phonon modes, also indicating that the collective lattice response is governed by spin correlations. These findings establish NCGO as a model system for investigating cooperative spin-lattice coupling and critical scaling behavior of phonon dynamics in low-dimensional magnetic materials.
In this work diverse results obtained from a number of low-dimensional quantum spin systems using Raman spectroscopy have been presented. The main motivation of this thesis is to hunt for new types of elementary excitations which may be present in low-dimensional spin systems with exotic spin topology. The studied systems can be on the one hand characterized by the formation of spin dimers which originate from a special spin topology like ACuCl3 (A=Tl, K), LiCu2O2, and SrCu(BO3)2. On the other hand, the system such as K2V3O8 and Cu2Te2O5X2 (X=Br,Cl) is dominated by quantum fluctuations due to reduced dimensionalilty. A powerful tool for studying low-dimensional spin systems is Raman spectroscopy which is sensitive to nearly all possible types of collective excitations as well as the interplay among them. In particular, magnetic light scattering can provide information about exchange paths and coupling constants, spinon excitations, spin gaps, and triplet-triplet interactions. The main results are summarized as follows; (i) the observation of a coherent coexistence of long-rang order and dimerized state in the frustrated spin chain system LiCu2O2, (ii) the presence of three-magnon scattering and dynamic spin-phonon coupling in the three-dimensional coupled spin dimer systems ACuCl3 (A=Tl, K), (iii) anomalous low-energy excitations including two-magnon scattering and electronic/orbital excitations in the two-dimensional Heisenberg antiferromagnetic system K2V3O8, (iv) the observation of inter-plane soft mode and a coupling of spin to soft mode in the quasi two-dimensional orthogonal dimer system SrCu(BO3)2, and (v) the existence of longitudinal magnons in the spin tetrahedra system Cu2Te2O5X2 (X=Br,Cl).
Abstract Motivated by recent advancements in theoretical and experimental studies of the high-energy excitations on an antiferromagnetic trimer chain, we numerically investigate the quantum phase transition and composite dynamics in this system by applying a magnetic field. The numerical methods we used include the exact diagonalization, density matrix renormalization group, time-dependent variational principle, and cluster perturbation theory. From calculating the entanglement entropy, we have revealed the phase diagram which includes the XY-I, 1/3 magnetization plateau, XY-II, and ferromagnetic phases. Both the critical XY-I and XY-II phases are characterized by the conformal field theory with a central charge c ≃ 1. By analyzing the dynamic spin structure factor, we elucidate the distinct features of spin dynamics across different phases. In the regime with weak intertrimer interaction, we identify the intermediate-energy and high-energy modes in the XY-I and 1/3 magnetization plateau phases as internal trimer excitations, corresponding to the propagating of doublons and quartons, respectively. Notably, applying a magnetic field splits the high-energy spectrum into two branches, labeled as the upper quarton and lower quarton. Furthermore, we explore the spin dynamics of a frustrated trimerized model closely related to the quantum magnet Na 2 Cu 3 Ge 4 O 12 . In the end, we extend our discuss on the possibility of the quarton Bose-Einstein condensation in the trimer systems. Our results are expected to be further verified through the inelastic neutron scattering and resonant inelastic X-ray scattering, and also provide valuable insights for exploring high-energy exotic excitations.
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.
Trimerized Spin-1/2 Chain: Emergent Low-Energy Hamiltonian, Higher-Energy Excitations, and Magnetic and Thermodynamic Responses
We investigate a spin-1/2 antiferromagnetic chain with trimerized exchange couplings relevant to Na2Cu3Ge4O12. We show that the low-energy Hilbert space maps onto an effective Heisenberg chain of composite spin-1/2 trimer degrees of freedom with positive coupling, enabling an exact spinon excitations via the Bethe ansatz. To access higher-energy dynamics, we develop a self-consistent Jordan-Wigner mean-field theory that yields three fermionic bands reflecting the underlying trimer structure. Remarkably, this approach reproduces the exact low-energy spinon continuum while predicting two additional higher-energy excitation bands consistent with the experimental observations and previous numerical simulations. The theory further captures the 1/3 magnetization plateau under an applied magnetic field, and provides testable predictions in magnetic susceptibility and specific heat. Our results establish a unified framework connecting low- and high-energy excitations in trimerized quantum spin chains.
The novel quantum magnet BaCu2V2O8 was recently discovered to be a rare physical realization of a one-dimensional antiferromagnetic-ferromagnetic dimerized chain which displays strongly correlated phenomena at elevated temperatures [E. S. Klyushina et al., Phys. Rev. B 93, 241109(R) (2016)]. This paper presents an extended study of the Hamiltonian of BaCu2V2O8 at base temperature. Static susceptibility and inelastic neutron scattering data are compared to several theoretical models. An analytical relation for the dynamic structure factor of the complex unit cell of BaCu2V2O8 is derived and used to identify the intrachain exchange paths. Further analysis using the first moment of the dynamic structure factor was employed to determine the exchange path responsible for the intradimer interaction. This analysis reveals that the dimer chain is formed by a dominant antiferromagnetic exchange interaction Jintra=40.92meV which is realized via the Cu-O-V(II)-O-Cu superexchange path and a weak ferromagnetic coupling ${J}_{\mathrm{inter}}=\ensuremath{-}11.97$ meV which arises within the copper-oxygen double plaquettes.