Ch. Rüegg

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.

Quantum and classical criticality in a dimerized quantum antiferromagnet

A quantum critical point (QCP) is a singularity in the phase diagram arising because of 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 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.

Direct Observation of Magnon Fractionalization in the Quantum Spin Ladder

We measure by inelastic neutron scattering the spin excitation spectra as a function of applied magnetic field in the quantum spin-ladder material (C5H12N)2CuBr4. Discrete magnon modes at low fields in the quantum disordered phase and at high fields in the saturated phase contrast sharply with a spinon continuum at intermediate fields characteristic of the Luttinger-liquid phase. By tuning the magnetic field, we drive the fractionalization of magnons into spinons and, in this deconfined regime, observe both commensurate and incommensurate continua.

Pressure dependence of the magnetic order in CrAs: A neutron diffraction investigation

The suppression of magnetic order with pressure concomitant with the appearance of pressure-induced superconductivity was recently discovered in CrAs. Here we present a neutron diffraction study of the pressure evolution of the helimagnetic ground state towards and in the vicinity of the superconducting phase. Neutron diffraction on polycrystalline CrAs was employed from zero pressure to 0.65 GPa and at various temperatures. The helimagnetic long-range order is sustained under pressure and the magnetic propagation vector does not show any considerable change. The average ordered magnetic moment is reduced from 1.73(2) mu(B) at ambient pressure to 0.4(1) mu(B) close to the critical pressure P-c approximate to 0.7 GPa, at which magnetic order is completely suppressed. The width of the magnetic Bragg peaks strongly depends on temperature and pressure, showing a maximum in the region of the onset of superconductivity. We interpret this as associated with competing ground states in the vicinity of the superconducting phase.

Spin-orbit-induced orbital excitations in Sr2RuO4 and Ca2RuO4: A resonant inelastic x-ray scattering study

High-resolution resonant inelastic x-ray scattering (RIXS) at the oxygen K edge has been used to study the orbital excitations of Ca2RuO4 and Sr2RuO4. In combination with linear dichroism x-ray absorption spectroscopy, the ruthenium 4d-orbital occupation and excitations were probed through their hybridization with the oxygen p orbitals. These results are described within a minimal model, taking into account crystal field splitting and a spin-orbit coupling λso=200 meV. The effects of spin-orbit interaction on the electronic structure and implications for the Mott and superconducting ground states of (Ca,Sr)2RuO4 are discussed.

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. The more complex spin Hamiltonian revealed in our study leads to a distinct form of magnon Bose-Einstein condensate phase with a spatially modulated condensate amplitude.

Strong coupling of Sm and Fe magnetism in SmFeAsO as revealed by magnetic x-ray scattering

The magnetic structures adopted by the Fe and Sm sublattices in SmFeAsO have been investigated using element-specific x-ray resonant and nonresonant magnetic scattering techniques. Between 110 and 5 K, the Sm and Fe moments are aligned along the c and a directions, respectively, according to the same magnetic representation Gamma(5) and the same propagation vector (1 0 1/2). Below 5 K, the magnetic order of both sublattices changes to a different magnetic structure, and the Sm moments reorder in a magnetic unit cell equal to the chemical unit cell. Modeling of the temperature dependence for the Sm sublattice, as well as a change in the magnetic structure below 5 K, provides clear evidence of a surprisingly strong coupling between the two sublattices, and indicates the need to include anisotropic exchange interactions in models of SmFeAsO and related compounds.

Anisotropy of magnetic interactions in the spin-ladder compound (C5H12N)2CuBr4

Magnetic excitations in the spin-ladder material (C5H12N)2CuBr4 [BPCB] are probed by highresolution multi-frequency electron spin resonance (ESR) spectroscopy. Our experiments provide a direct evidence for a biaxial anisotropy (� 5% of the dominant exchange interaction), that is in contrast to a fully isotropic spin-ladder model employed for this system previously. It is argued that this anisotropy in BPCB is caused by spin-orbit coupling, which appears to be important for describing magnetic properties of this compound. The zero-field zone-center gap in the excitation spectrum of BPCB, �0/kB = 16.5 K, is detected directly. Furthermore, an ESR signature of the inter-ladder exchange interactions is obtained. The detailed characterization of the anisotropy in BPCB completes the determination of the full spin hamiltonian of this exceptional spin-ladder material and shows ways to study anisotropy effects in spin ladders.

Quantum Statistics of Interacting Dimer Spin Systems

The compound TlCuCl(3) 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 Würtz [Phys. Rev. B 50, 13 515 (1994)10.1103/Phys. Rev. B 50, 13515] provides an appropriate quantum statistical model for dimer spin systems at finite temperatures, where many-body correlations become particularly important.

Inelastic x-ray scattering study of superconducting SmFeAsO1-xFy single crystals: Evidence for strong momentum-dependent doping-induced renormalizations of optical phonons

We report inelastic x-ray scattering experiments on the lattice dynamics in SmFeAsO and superconducting SmFeAsO0.60F0.35 single crystals. Particular attention was paid to the dispersions along the [100] direction of three optical modes close to 23 meV, polarized out of the FeAs planes. Remarkably, two of these modes are strongly renormalized upon fluorine doping. These results provide significant insight into the energy and momentum dependence of the coupling of the lattice to the electron system and underline the importance of spin-phonon coupling in the superconducting iron pnictides.