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

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

Neutron Scattering Study of Magnetic Ordering and Excitations in the Doped Spin Gap System Tl(Cu1−x_{1-x}Mgx_x)Cl3_3

Neutron elastic and inelastic scattering measurements have been performed in order to investigate the spin structure and the magnetic excitations in the impurity-induced antiferromagnetic ordered phase of the doped spin gap system Tl(Cu$_{1-x}$Mg$_x$)Cl$_3$ with $x=0.03$. The magnetic Bragg reflections indicative of the ordering were observed at ${\pmb Q}=(h, 0, l)$ with integer $h$ and odd $l$ below $T_{\rm N}=3.45$ K. It was found that the spin structure of the impurity-induced antiferromagnetic ordered phase on average in Tl(Cu$_{1-x}$Mg$_x$)Cl$_3$ with $x=0.03$ is the same as that of the field-induced magnetic ordered phase for ${\pmb H} \parallel b$ in the parent compound TlCuCl$_3$. The triplet magnetic excitation was clearly observed in the $a^*$-$c^*$ plane and the dispersion relations of the triplet excitation were determined along four different directions. The lowest triplet excitation corresponding to the spin gap was observed at ${\pmb Q}=(h, 0, l)$ with integer $h$ and odd $l$, as observed in TlCuCl$_3$. It was also found that the spin gap increases steeply below $T_{\rm N}$ upon decreasing temperature. This strongly indicates that the impurity-induced antiferromagnetic ordering coexists with the spin gap state in Tl(Cu$_{1-x}$Mg$_x$)Cl$_3$ with $x=0.03$.Comment: 24 pages, 7 figures, 11 eps files, revtex style, will appear in Phys. Rev.

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

Impurity-Induced Antiferromagnetic Ordering in the Spin Gap System TlCuCl_3

The magnetization measurements have been performed on the doped spin gap system TlCu_{1-x}Mg_xCl_3 with x <= 0.025. The parent compound TlCuCl_3 is a three-dimensional coupled spin dimer system with the excitation gap Delta/k_B = 7.7 K. The impurity-induced antiferromagnetic ordering was clearly observed. The easy axis lies in the (0,1,0) plane. It was found that the transition temperature increases with increasing Mg^{2+} concentration x, while the spin-flop transition field is almost independent of x. The magnetization curve suggests that the impurity-induced antiferromagnetic ordering coexists with the spin gap for x <= 0.017.Comment: 5 pages, 6 figures, revtex styl

Field-Induced Magnetic Order in Quantum Spin Liquids

We study magnetic field-induced three-dimensional ordering transitions in low-dimensional quantum spin liquids, such as weakly coupled, antiferromagnetic spin-1/2 Heisenberg dimers and ladders. Using stochastic series expansion quantum Monte Carlo simulations, thermodynamic response functions are obtained down to ultra-low temperatures. We extract the critical scaling exponents which dictate the power-law dependence of the transition temperature on the applied magnetic field. These are compared with recent experiments on candidate materials and with predictions for the Bose-Einstein condensation of magnons obtained in mean-field theory.Comment: RevTex, 4 pages with 5 figure

Magnetization plateaux in dimerized spin ladder arrays

We investigate the ground state magnetization plateaux appearing in spin 1/2 two-leg ladders built up from dimerized antiferromagnetic Heisenberg chains and dimerized zig-zag interchain couplings. Using both Abelian bosonization and Lanczos methods we find that the system yields rather unusual plateaux and exhibits massive and massless phases for specific choices or ``tuning'' of exchange interactions. The relevance of this behavior in the study of NH_4CuCl_3 is discussed.Comment: 9 pages, RevTeX, 11 postscript figure

Drastic Change of Magnetic Phase Diagram in Doped Quantum Antiferromagnet TlCu1−x_{1-x}Mgx_xCl3_3

TlCuCl$_3$ is a coupled spin dimer system, which has a singlet ground state with an excitation gap of $\Delta/g\mu_{\mathrm B}$ = 5.5 T. TlCu$_{1-x}$Mg$_x$Cl$_3$ doped with nonmagnetic Mg$^{2+}$ ions undergoes impurity-induced magnetic ordering. Because triplet excitation with a finite gap still remains, this doped system can also undergo magnetic-field-induced magnetic ordering. By specific heat measurements and neutron scattering experiments under a magnetic field, we investigated the phase diagram in TlCu$_{1-x}$Mg$_x$Cl$_3$ with $x\sim 0.01$, and found that impurity- and field-induced ordered phases are the same. The gapped spin liquid state observed in pure TlCuCl$_3$ is completely wiped out by the small amount of doping.Comment: 9 pages, 5 figures, jpsj2 class file, to be published in J. Phy. Soc. Jpn. Vol.75 No.3 (2006); layout changed, unrelated figure remove

Excitation Spectra of Structurally Dimerized and Spin-Peierls Chains in a Magnetic Field

The dynamical spin structure factor and the Raman response are calculated for structurally dimerized and spin-Peierls chains in a magnetic field, using exact diagonalization techniques. In both cases there is a spin liquid phase composed of interacting singlet dimers at small fields h < h_c1, an incommensurate regime (h_c1 < h < h_c2) in which the modulation of the triplet excitation spectra adapts to the applied field, and a fully spin polarized phase above an upper critical field h_c2. For structurally dimerized chains, the spin gap closes in the incommensurate phase, whereas spin-Peierls chains remain gapped. In the spin liquid regimes, the dominant feature of the triplet spectra is a one-magnon bound state, separated from a continuum of states at higher energies. There are also indications of a singlet bound state above the one-magnon triplet.Comment: RevTex, 10 pages with 8 eps figure

Three-Dimensional Ordering in Weakly Coupled Antiferromagnetic Ladders and Chains

A theoretical description is presented for low-temperature magnetic-field induced three-dimensional (3D) ordering transitions in strongly anisotropic quantum antiferromagnets, consisting of weakly coupled antiferromagnetic spin-1/2 chains and ladders. First, effective continuum field theories are derived for the one-dimensional subsystems. Then the Luttinger parameters, which determine the low-temperature susceptibilities of the chains and ladders, are calculated from the Bethe ansatz solution for these effective models. The 3D ordering transition line is obtained using a random phase approximation for the weak inter-chain (inter-ladder) coupling. Finally, considering a Ginzburg criterion, the fluctuation corrections to this approach are shown to be small. The nature of the 3D ordered phase resembles a Bose condensate of integer-spin magnons. It is proposed that for systems with higher spin degrees of freedom, e.g. N-leg spin-1/2 ladders, multi-component condensates can occur at high magnetic fields.Comment: RevTex, 18 pages with 7 figure