Dimensional reduction by pressure in the magnetic framework material CuF2_{2}(D2_{2}O)2_{2}pyz: from spin-wave to spinon excitations

Metal organic magnets have enormous potential to host a variety of electronic and magnetic phases that originate from a strong interplay between the spin, orbital and lattice degrees of freedom. We control this interplay in the quantum magnet CuF$_2$(D$_2$O)$_2$pyz by using high pressure to drive the system through a structural and magnetic phase transition. Using neutron scattering, we show that the low pressure state, which hosts a two-dimensional square lattice with spin-wave excitations and a dominant exchange coupling of 0.89 meV, transforms at high pressure into a one-dimensional spin-chain hallmarked by a spinon continuum and a reduced exchange interaction of 0.43 meV. This direct microscopic observation of a magnetic dimensional crossover as a function of pressure opens up new possibilities for studying the evolution of fractionalised excitations in low dimensional quantum magnets and eventually pressure-controlled metal--insulator transitions

Neutron scattering study of the field-dependent ground state and the spin dynamics in S=1/2 NH4CuCl3

Elastic and inelastic neutron scattering experiments have been performed on the dimer spin system NH4CuCl3, which shows plateaus in the magnetization curve at m=1/4 and m=3/4 of the saturation value. Two structural phase transitions at T1≈156  K and at T2=70  K lead to a doubling of the crystallographic unit cell along the b direction and as a consequence a segregation into different dimer subsystems. Long-range magnetic ordering is reported below TN=1.3  K. The magnetic field dependence of the excitation spectrum identifies successive quantum phase transitions of the dimer subsystems as the driving mechanism for the unconventional magnetization process in agreement with a recent theoretical model

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

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

Spinon localization in the heat transport of the spin-1/2 ladder compound (C5_5H12_{12}N)2_2CuBr4_4

We present experiments on the magnetic field-dependent thermal transport in the spin-1/2 ladder system (C$_5$H$_{12}$N)$_2$CuBr$_4$. The thermal conductivity $\kappa(B)$ is only weakly affected by the field-induced transitions between the gapless Luttinger-liquid state realized for $B_{c1}< B < B_{c2}$ and the gapped states, suggesting the absence of a direct contribution of the spin excitations to the heat transport. We observe, however, that the thermal conductivity is strongly suppressed by the magnetic field deeply within the Luttinger-liquid state. These surprising observations are discussed in terms of localization of spinons within finite ladder segments and spinon-phonon umklapp scattering of the predominantly phononic heat transport.Comment: 4 pages, 3 figure

Microscopic model for the magnetization plateaus in NH4CuCl3

A simple model consisting of three distinct dimer sublattices is proposed to describe the magnetism of NH4CuCl3. It explains the occurrence of magnetization plateaus only at 1/4 and 3/4 of the saturation magnetization. The field dependence of the excitation modes observed by ESR measurements is also explained by the model. The model predicts that the magnetization plateaus should disappear under high pressure.Comment: 4 pages, 5 figures, REVTeX

Pressure-induced electronic phase separation of magnetism and superconductivity in CrAs

The recent discovery of pressure induced superconductivity in the binary helimagnet CrAs has attracted much attention. How superconductivity emerges from the magnetic state and what is the mechanism of the superconducting pairing are two important issues which need to be resolved. In the present work, the suppression of magnetism and the occurrence of superconductivity in CrAs as a function of pressure ($p$) were studied by means of muon spin rotation. The magnetism remains bulk up to $p\simeq3.5$~kbar while its volume fraction gradually decreases with increasing pressure until it vanishes at $p\simeq$7~kbar. At 3.5 kbar superconductivity abruptly appears with its maximum $T_c \simeq 1.2$~K which decreases upon increasing the pressure. In the intermediate pressure region ($3.5\lesssim p\lesssim 7$~kbar) the superconducting and the magnetic volume fractions are spatially phase separated and compete for phase volume. Our results indicate that the less conductive magnetic phase provides additional carriers (doping) to the superconducting parts of the CrAs sample thus leading to an increase of the transition temperature ($T_c$) and of the superfluid density ($\rho_s$). A scaling of $\rho_s$ with $T_c^{3.2}$ as well as the phase separation between magnetism and superconductivity point to a conventional mechanism of the Cooper-pairing in CrAs.Comment: 9 pages, 8 figure

Role of multiple subband renormalization in the electronic transport of correlated oxide superlattices

Metallic behavior of band-insulator/ Mott-insulator interfaces was observed in artificial perovskite superlattices such as in nanoscale SrTiO3/LaTiO3 multilayers. Applying a semiclassical perspective to the parallel electronic transport we identify two major ingredients relevant for such systems: i) the quantum confinement of the conduction electrons (superlattice modulation) leads to a complex, quasi-two dimensional subband structure with both hole- and electron-like Fermi surfaces. ii) strong electron-electron interaction requires a substantial renormalization of the quasi-particle dispersion. We characterize this renormalization by two sets of parameters, namely, the quasi-particle weight and the induced particle-hole asymmetry of each partially filled subband. In our study, the quasi-particle dispersion is calculated self-consistently as function of microscopic parameters using the slave-boson mean-field approximation introduced by Kotliar and Ruckenstein. We discuss the consequences of strong local correlations on the normal-state free-carrier response in the optical conductivity and on the thermoelectric effects.Comment: 11 pages, 4 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