arXiv:0709.3632 · Proceedings of the National Academy of Sciences
Quantum dynamics and entanglement of spins on a square lattice
Niels Bech Christensen, Henrik Moodysson Rønnow, MCMORROW Desmond Francis, Andrew Harrison, T. G. Perring, M. Enderle, R. Coldea, L. P. Régnault, G. Aeppli
Bulk magnetism in solids is fundamentally quantum mechanical in nature. Yet in many situations, including our everyday encounters with magnetic materials, quantum effects are masked, and it often suffices to think of magnetism in terms of the interaction between classical dipole moments. Whereas this intuition generally holds for ferromagnets, even as the size of the magnetic moment is reduced to that of a single electron spin (the quantum limit), it breaks down spectacularly for antiferromagnets, particularly in low dimensions. Considerable theoretical and experimental progress has been made in understanding quantum effects in one-dimensional quantum antiferromagnets, but a complete experimental description of even simple two-dimensional antiferromagnets is lacking. Here we describe a comprehensive set of neutron scattering measurements that reveal a non-spin-wave continuum and strong quantum effects, suggesting entanglement of spins at short distances in the simplest of all two-dimensional quantum antiferromagnets, the square lattice Heisenberg system.
Bulk magnetism in solids is fundamentally quantum mechanical in nature. Yet in many situations, including our everyday encounters with magnetic materials, quantum effects are masked, and it often suffices to think of magnetism in terms of the interaction between classical dipole moments. Whereas this intuition generally holds for ferromagnets, even as the size of the magnetic moment is reduced to that of a single electron spin (the quantum limit), it breaks down spectacularly for antiferromagnets, particularly in low dimensions. Considerable theoretical and experimental progress has been made in understanding quantum effects in one-dimensional quantum antiferromagnets, but a complete experimental description of even simple two-dimensional antiferromagnets is lacking. Here we describe a comprehensive set of neutron scattering measurements that reveal a non-spin-wave continuum and strong quantum effects, suggesting entanglement of spins at short distances in the simplest of all two-dimensional quantum antiferromagnets, the square lattice Heisenberg system.
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.
Spin waves (magnons) in two dimensions are the potential glue in high-temperature superconductors so that their quantitative understanding is mandatory. Yet even for the fundamental case of the undoped Heisenberg model on the square lattice a consistent picture is still lacking. Significant spectral continua are taken as evidence of the existence of fractional excitations (spinons), but descriptions in terms of spinons fail to show the established absence of an energy gap. Here a fully consistent picture of the dynamics in the square-lattice quantum antiferromagnet is provided which agrees with the experimental findings. The key step is to capture (i) the strong attractive interaction between the spin waves and (ii) the vertex corrections of the observables.
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.
Low dimensional quantum magnets which display a collective singlet ground state and a gap in their magnetic excitation spectrum provide a framework for much exotic phase behavior in new materials, with high temperature superconductivity being the best appreciated example. Neutron scattering techniques can be applied to study a wide variety of problems in condensed matter physics. These techniques are particularly useful as applied to understanding the magnetic properties of quantum magnets that display exotic phases. SrCu2(BO3)2, is a rare example of a two-dimensional quantum magnet for which an exact theoretical solution describing its ground state is known to be a collective singlet. Previous high resolution neutron scattering measurements identified the most prominent features of the spin excitation spectrum in SrCu2(BO3)2, including the presence of one and two triplet excitations and weak dispersion characteristic of subleading terms in the spin Hamiltonian. The resemblance between the spin gap behavior in the Mott insulator SrCu2(BO3)2 and that associated with high temperature superconductors motivated the consideration of the significance of doping in order to understand the properties of this quantum magnetic system. For this reason, a series of neutron scattering studies on doped SrCu2(BO3)2 were initiated. These series of investigations began with the performance of neutron scattering measurements on a SrCu(2-x)Mgx(BO3)2 single crystal in order to introduce magnetic vacancies to the system. These results revealed the presence of new spin excitations within the singlet-triplet gap of this system. Application of a magnetic field induces Zeeman-split states associated with un-paired spins which exist as a consequence of doping with quenched non-magnetic impurities. Additional substantial broadening of both the one and two triplet excitations is observed in the doped system as compared to the pure system. Theoretical calculations are shown to qualitatively account for these features. These studies were extended to neutron scattering measurements on Sr(1-x)LaxCu2(BO3)2, with an aim of introducing charged carriers into this system. The broadening of the one and two triplet excitations is observed and compared to the thermally induced finite lifetime of the pure system. The temperature dependence of this broadening in Sr(1-x)LaxCu2(BO3)2 is different compared to that observed in both SrCu2(BO3)2 and SrCu(2-x)Mgx(BO3)2. It has also been suggested that there is a relation between the spin-lattice interaction in SrCu2(BO3)2 and the magnetic dynamics at low temperatures and high magnetic fields. For this reason there has been increased interest in the study of the crystalline structure and vibrational modes of SrCu2(BO3)2. In order to investigate the role of the lattice in the formation of the singlet ground state in SrCu2(BO3)2, a series of low and high energy neutron scattering measurements were carried out on this system to study both the crystalline structure as well as the normal modes of vibration of the lattice, the transverse acoustic and optical phonons. Transverse acoustic phonons with energies comparable to and higher than the onset of the two triplet continuum show substantially increased lifetimes on entering the singlet ground state below ~ 10 K. This may indicate the removal of the decay channel for the phonons due to the gapping of the spin excitation spectrum in SrCu2(BO3)2 at low temperatures. In high energy inelastic neutron scattering we observe broadening of optic phonons in the ~ 52 to 65 meV region on entering the low temperature singlet ground state. Additionally, the magnetic properties of CuMoO4, which is a triclinic quantum magnet system based on S=1/2 moments at the Cu2+ site, were studied using elastic and inelastic neutron scattering experiments. This material exhibits a first order structural phase transition at ~ 190 K as well as a magnetic phase transition at ~ 1.75 K. We were primarily interested in the low temperature magnetic properties of this material. Magnetization and heat capacity measurements as well as elastic and inelastic neutron scattering measurements were conducted on this system within the low temperature ordered phase. These studies confirm that this material has a magnetic phase transition at ~ 1.7 K. Neutron scattering results indicate that this magnetically ordered phase is characterized by a doubling of the a axis. Inelastic neutron scattering measurements revealed a gapped magnetic excitation spectrum in zero magnetic field, which could be filled in by the application of magnetic fields approaching 7 T.
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.
Molecular magnets are ideal systems to probe the realm that borders quantum and classical physics, as well as to study decoherence phenomena in nanoscale systems. The control of the quantum behavior of these materials and their structural characteristics requires synthesis of new complexes with desirable properties which will allow probing of the fundamental aspects of nanoscale physics and quantum information processing. Of particular interest among the magnetic molecular materials are single-molecule magnets (SMMs) and antiferromagnetic (AFM) molecular wheels in which the spin state of the molecule is known to behave quantum mechanically at low temperatures. In previous experiments the dynamics of the magnetic moment of the molecules is governed by incoherent quantum tunneling. Short decoherence times are mainly due to interactions between molecular magnets within the crystal and interactions of the electronic spin with the nuclear spin of neighboring ions within the molecule. This decoherence problem has imposed a limit to the understanding of the molecular spin dynamics and the sources of decoherence in condensed matter systems. Particularly, intermolecular dipolar interactions within the crystal, which shorten the coherence times in concentrated samples, have stymied progress in this direction. Several recent works have reported a direct measurement of the decoherence time in molecular magnets. This has been done by eliminating the dephasing created by dipolar interactions between neighboring molecules. This has been achieved by a) a dilution of the molecules in a liquid solution to decrease the dipolar interaction by separating the molecules, and b) by polarizing the spin bath by applying a high magnetic field at low temperatures. Unfortunately, both approaches restrict the experimental studies of quantum dynamics. For example, the dilution of molecular magnets in liquid solution causes a dispersion of the molecular spin orientation and anisotropy axes, while the large fields required to polarize the spin bath overcome the anisotropy of the molecular spin. In this thesis I have explored two methods to overcome dipolar interactions in molecular magnets: a) studying the dynamics of molecular magnets in single crystals where the separation between magnetic molecules is obtained by chemical doping or where the high crystalline quality allows observations intrinsic to the quantum mechanical nature of the tunneling of the spin, and b) studying the electronic transport through an individual magnetic molecule which has been carefully placed in a single-electron transistor device. I have used EPR microstrip resonators to measure Fe17Ga molecular wheels within single crystals of Fe18 AFM wheels, as well as demonstrating, for the first time in a Single Molecule Magnet, the complete suppression of a Quantum Tunneling of the Magnetization transition forbidden by molecular symmetry.