Dynamical Structure Factors for Dimerized Spin Systems

We discuss the transition strength between the disordered ground state and the basic low-lying triplet excitation for interacting dimer materials by presenting theoretical calculations and series expansions as well as inelastic neutron scattering results for the material KCuCl_3. We describe in detail the features resulting from the presence of two differently oriented dimers per unit cell and show how energies and spectral weights of the resulting two modes are related to each other. We present results from the perturbation expansion in the interdimer interaction strength and thus demonstrate that the wave vector dependence of the simple dimer approximation is modified in higher orders. Explicit results are given in 10th order for dimers coupled in 1D, and in 2nd order for dimers coupled in 3D with application to KCuCl_3 and TlCuCl_3.Comment: 17 pages, 6 figures, part 2 is based on cond-mat/021133

Random Bond Effect in the Quantum Spin System (Tl1−x_{1-x}Kx_{x})CuCl3_3

The effect of exchange bond randomness on the ground state and the field-induced magnetic ordering was investigated through magnetization measurements in the spin-1/2 mixed quantum spin system (Tl$_{1-x}$K$_{x}$)CuCl$_3$ for $x<0.36$. Both parent compounds TlCuCl$_3$ and KCuCl$_3$ are coupled spin dimer systems, which have the singlet ground state with excitation gaps ${\Delta}/k_{\rm B}=7.7$ K and 31 K, respectively. Due to bond randomness, the singlet ground state turns into the magnetic state with finite susceptibility, nevertheless, the excitation gap remains. Field-induced magnetic ordering, which can be described by the Bose condensation of excited triplets, magnons, was observed as in the parent systems. The phase transition temperature is suppressed by the bond randomness. This behavior may be attributed to the localization effect.Comment: 19 pages, 7 figures, 12 eps files, revtex, will appear in PR

Field-Induced Magnetic Ordering in the Quantum Spin System KCuCl3_3

KCuCl$_3$ is a three-dimensional coupled spin-dimer system and has a singlet ground state with an excitation gap ${\Delta}/k_{\rm B}=31$ K. High-field magnetization measurements for KCuCl$_3$ have been performed in static magnetic fields of up to 30 T and in pulsed magnetic fields of up to 60 T. The entire magnetization curve including the saturation region was obtained at $T=1.3$ K. From the analysis of the magnetization curve, it was found that the exchange parameters determined from the dispersion relations of the magnetic excitations should be reduced, which suggests the importance of the renormalization effect in the magnetic excitations. The field-induced magnetic ordering accompanied by the cusplike minimum of the magnetization was observed as in the isomorphous compound TlCuCl$_3$. The phase boundary was almost independent of the field direction, and is represented by the power law. These results are consistent with the magnon Bose-Einstein condensation picture for field-induced magnetic ordering.Comment: 9 pages, 7 figures, 9 eps files, revtex styl

Ehrenfest relations and magnetoelastic effects in field-induced ordered phases

Magnetoelastic properties in field-induced magnetic ordered phases are studied theoretically based on a Ginzburg-Landau theory. A critical field for the field-induced ordered phase is obtained as a function of temperature and pressure, which determine the phase diagram. It is found that magnetic field dependence of elastic constant decreases discontinuously at the critical field, Hc, and that it decreases linearly with field in the ordered phase (H>Hc). We found an Ehrenfest relation between the field dependence of the elastic constant and the pressure dependence of critical field. Our theory provides the theoretical form for magnetoelastic properties in field- and pressure-induced ordered phases.Comment: 7 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 Magnetic Quantum Phase Transition in Gapped Spin System KCuCl3

Magnetization and neutron elastic scattering measurements under a hydrostatic pressure were performed on KCuCl3, which is a three-dimensionally coupled spin dimer system with a gapped ground state. It was found that an intradimer interaction decreases with increasing pressure, while the sum of interdimer interactions increases. This leads to the shrinkage of spin gap. A quantum phase transition from a gapped state to an antiferromagnetic state occurs at Pc ? 8.2 kbar. For P > P c, magnetic Bragg reflections were observed at reciprocal lattice points equivalent to those for the lowest magnetic excitation at zero pressure. This confirms that the spin gap decreases and closes under applied pressure.Comment: 7 pages, 10 figures, submitted to J. Phys. Soc. Jp

The disordered-free-moment phase: a low-field disordered state in spin-gap antiferromagnets with site dilution

Site dilution of spin-gapped antiferromagnets leads to localized free moments, which can order antiferromagnetically in two and higher dimensions. Here we show how a weak magnetic field drives this order-by-disorder state into a novel disordered-free-moment phase, characterized by the formation of local singlets between neighboring moments and by localized moments aligned antiparallel to the field. This disordered phase is characterized by the absence of a gap, as it is the case in a Bose glass. The associated field-driven quantum phase transition is consistent with the universality of a superfluid-to-Bose-glass transition. The robustness of the disordered-free-moment phase and its prominent features, in particular a series of pseudo-plateaus in the magnetization curve, makes it accessible and relevant to experiments.Comment: 4 pages, 4 figure

Spin-resonance modes of the spin-gap magnet TlCuCl_3

Three kinds of magnetic resonance signals were detected in crystals of the spin-gap magnet TlCuCl_3. First, we have observed the microwave absorption due to the excitation of the transitions between the singlet ground state and the excited triplet states. This mode has the linear frequency-field dependence corresponding to the previously known value of the zero-field spin-gap of 156 GHz and to the closing of spin-gap at the magnetic field H_c of about 50 kOe. Second, the thermally activated resonance absorption due to the transitions between the spin sublevels of the triplet excitations was found. These sublevels are split by the crystal field and external magnetic field. Finally, we have observed antiferromagnetic resonance absorption in the field-induced antiferromagnetic phase above the critical field H_c. This resonance frequency is strongly anisotropic with respect to the direction of the magnetic field.Comment: v.2: typo correction (one of the field directions was misprinted in the v.1

Dispersive magnetic excitations in the S=1 antiferromagnet Ba3_3Mn2_2O8_8

We present powder inelastic neutron scattering measurements of the S=1 dimerized antiferromagnet Ba$_3$Mn$_2$O$_8$. The $T=1.4$ K magnetic spectrum exhibits a spin-gap of $\Delta \approx 1.0$ meV and a dispersive spectrum with a bandwidth of approximately 1.5 meV. Comparison to coupled dimer models describe the dispersion and scattering intensity accurately and determine the exchange constants in Ba$_3$Mn$_2$O$_8$. The wave vector dependent scattering intensity confirms the proposed S=1 dimer bond. Temperature dependent measurements of the magnetic excitations indicate the presence of both singlet-triplet and thermally activated triplet-quintet excitations.Comment: 8 pages, 8 figures, Submitted to Physical Review B, Resubmited versio