Complete bond-operator theory of the two-chain spin ladder

The discovery of the almost ideal, two-chain spin-ladder material (C_5H_12N)_2CuBr_4 has once again focused attention on this most fundamental problem in low-dimensional quantum magnetism. Within the bond-operator framework, three qualitative advances are introduced which extend the theory to all finite temperatures and magnetic fields in the gapped regime. This systematic description permits quantitative and parameter-free experimental comparisons, which are presented for the specific heat, and predictions for thermal renormalization of the triplet magnon excitations.Comment: 12 pages, 10 figure

Quantum Statistics of Interacting Dimer Spin Systems

The compound TlCuCl3 represents a model system of dimerized quantum spins with strong interdimer interactions. We investigate the triplet dispersion as a function of temperature by inelastic neutron scattering experiments on single crystals. By comparison with a number of theoretical approaches we demonstrate that the description of Troyer, Tsunetsugu, and Wuertz [Phys. Rev. B 50, 13515 (1994)] provides an appropriate quantum statistical model for dimer spin systems at finite temperatures, where many-body correlations become particularly important.Comment: 4 pages, 4 figures, to appear in Physical Review Letter

Multiple Magnon Modes and Consequences for the Bose-Einstein Condensed Phase in BaCuSi2O6

The compound BaCuSi2O6 is a quantum magnet with antiferromagnetic dimers of S = 1/2 moments on a quasi-2D square lattice. We have investigated its spin dynamics by inelastic neutron scattering experiments on single crystals with an energy resolution considerably higher than in an earlier study. We observe multiple magnon modes, indicating clearly the presence of magnetically inequivalent dimer sites. This more complex spin Hamiltonian leads to a distinct form of magnon Bose-Einstein condensate (BEC) phase with a spatially modulated condensate amplitude.Comment: 5 pages, 4 figures, to be published in Phys. Rev. Let

Quantum and classical criticality in a dimerized quantum antiferromagnet

A quantum critical point (QCP) is a singularity in the phase diagram arising due to quantum mechanical fluctuations. The exotic properties of some of the most enigmatic physical systems, including unconventional metals and superconductors, quantum magnets, and ultracold atomic condensates, have been related to the importance of the critical quantum and thermal fluctuations near such a point. However, direct and continuous control of these fluctuations has been difficult to realize, and complete thermodynamic and spectroscopic information is required to disentangle the effects of quantum and classical physics around a QCP. Here we achieve this control in a high-pressure, high-resolution neutron scattering experiment on the quantum dimer material TlCuCl3. By measuring the magnetic excitation spectrum across the entire quantum critical phase diagram, we illustrate the similarities between quantum and thermal melting of magnetic order. We prove the critical nature of the unconventional longitudinal ("Higgs") mode of the ordered phase by damping it thermally. We demonstrate the development of two types of criticality, quantum and classical, and use their static and dynamic scaling properties to conclude that quantum and thermal fluctuations can behave largely independently near a QCP.Comment: 6 pages, 4 figures. Original version, published version available from Nature Physics websit

Bound states and field-polarized Haldane modes in a quantum spin ladder

The challenge of one-dimensional systems is to understand their physics beyond the level of known elementary excitations. By high-resolution neutron spectroscopy in a quantum spin ladder material, we probe the leading multiparticle excitation by characterizing the two-magnon bound state at zero field. By applying high magnetic fields, we create and select the singlet (longitudinal) and triplet (transverse) excitations of the fully spin-polarized ladder, which have not been observed previously and are close analogs of the modes anticipated in a polarized Haldane chain. Theoretical modelling of the dynamical response demonstrates our complete quantitative understanding of these states.Comment: 6 pages, 3 figures plus supplementary material 7 pages 5 figure

Thermodynamics of the Spin Luttinger-Liquid in a Model Ladder Material

The phase diagram in temperature and magnetic field of the metal-organic, two-leg, spin-ladder compound (C5H12N)2CuBr4 is studied by measurements of the specific heat and the magnetocaloric effect. We demonstrate the presence of an extended spin Luttinger-liquid phase between two field-induced quantum critical points and over a broad range of temperature. Based on an ideal spin-ladder Hamiltonian, comprehensive numerical modelling of the ladder specific heat yields excellent quantitative agreement with the experimental data across the complete phase diagram.Comment: 4 pages, 4 figures, updated refs and minor changes to the text, version accepted for publication in Phys. Rev. Let

Field- and pressure-induced magnetic quantum phase transitions in TlCuCl_3

Thallium copper chloride is a quantum spin liquid of S = 1/2 Cu^2+ dimers. Interdimer superexchange interactions give a three-dimensional magnon dispersion and a spin gap significantly smaller than the dimer coupling. This gap is closed by an applied hydrostatic pressure of approximately 2kbar or by a magnetic field of 5.6T, offering a unique opportunity to explore the both types of quantum phase transition and their associated critical phenomena. We use a bond-operator formulation to obtain a continuous description of all disordered and ordered phases, and thus of the transitions separating these. Both pressure- and field-induced transitions may be considered as the Bose-Einstein condensation of triplet magnon excitations, and the respective phases of staggered magnetic order as linear combinations of dimer singlet and triplet modes. We focus on the evolution with applied pressure and field of the magnetic excitations in each phase, and in particular on the gapless (Goldstone) modes in the ordered regimes which correspond to phase fluctuations of the ordered moment. The bond-operator description yields a good account of the magnetization curves and of magnon dispersion relations observed by inelastic neutron scattering under applied fields, and a variety of experimental predictions for pressure-dependent measurements.Comment: 20 pages, 17 figure

Quantum Magnets under Pressure: Controlling Elementary Excitations in TlCuCl3

We follow the evolution of the elementary excitations of the quantum antiferromagnet TlCuCl3 through the pressure-induced quantum critical point, which separates a dimer-based quantum disordered phase from a phase of long-ranged magnetic order. We demonstrate by neutron spectroscopy the continuous emergence in the weakly ordered state of a low-lying but massive excitation corresponding to longitudinal fluctuations of the magnetic moment. This mode is not present in a classical description of ordered magnets, but is a direct consequence of the quantum critical point.Comment: 4 pages, 4 figure

Irradiation of benzene molecules by ion-induced and light-induced intense fields

Benzene, with its sea of delocalized $\pi$-electrons in the valence orbitals, is identified as an example of a class of molecules that enable establishment of the correspondence between intense ion-induced and laser-light-induced fields in experiments that probe ionization dynamics in temporal regimes spanning the attosecond and picosecond ranges.Comment: 4 ps figure