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

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

Observation of Field-Induced Transverse N\'{e}el Ordering in the Spin Gap System TlCuCl3_3

Neutron elastic scattering experiments have been performed on the spin gap system TlCuCl$_3$ in magnetic fields parallel to the $b$-axis. The magnetic Bragg peaks which indicate the field-induced N\'{e}el ordering were observed for magnetic field higher than the gap field $H_{\rm g}\approx 5.5$ T at $Q=(h, 0, l)$ with odd $l$ in the $a^*-c^*$ plane. The spin structure in the ordered phase was determined. The temperature and field dependence of the Bragg peak intensities and the phase boundary obtained were discussed in connection with a recent theory which describes the field-induced N\'{e}el ordering as a Bose-Einstein condensation of magnons.Comment: 4 pages, 5 eps figures, jpsj styl

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

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.

Frustration-Induced Two Dimensional Quantum Disordered Phase in Piperazinium Hexachlorodicuprate

Piperazinium Hexachlorodicuprate (PHCC) is shown to be a frustrated quasi-two-dimensional quantum Heisenberg antiferromagnet with a gapped spectrum. Zero-field inelastic neutron scattering and susceptibility and specific heat measurements as a function of applied magnetic field are presented. At T = 1.5 K, the magnetic excitation spectrum is dominated by a single propagating mode with a gap, Delta = 1 meV, and bandwidth of approximately 1.8 meV in the (h0l) plane. The mode has no dispersion along the b* direction indicating that neighboring a-c planes of the triclinic structure are magnetically decoupled. The heat capacity shows a reduction of the gap as a function of applied magnetic field in agreement with a singlet-triplet excitation spectrum. A field-induced ordered phase is observed in heat capacity and magnetic susceptibility measurements for magnetic fields greater than H_c1 approximately equal to 7.5 Tesla. Analysis of the neutron scattering data reveals the important exchange interactions and indicates that some of these are highly frustrated.Comment: 13 pages with 14 figures, 7 pages of text, 6 pages of figures. Submitted to Phys. Rev. B 4/7/2001. email comments to [email protected] or [email protected]

Quantum Critical Point of the XY Model and Condensation of Field-Induced Quasiparticles in Dimer Compounds

The quantum critical point of the three-dimensional XY model in a symmetry-preserving field is investigated. The results of Monte Carlo simulations with the directed-loop algorithm show that the quantum critical behavior is characterized by the mean-field values of critical exponents. The system-size dependence of various quantities is compared to a simple field-theoretical argument that supports the mean-field scaling

Pressure-Induced Magnetic Quantum Phase Transitions from Gapped Ground State in TlCuCl3

Magnetization maesurements under hydrostatic pressure were performed on an S=1/2 coupled spin system TlCuCl3 with a gapped ground state under magnetic field H parallel to the [2,0,1] direction. With increasing applied pressure P, the gap decreases and closes completely at Pc=0.42 kbar. For P>Pc, TlCuCl3 undergoes antiferromagnetic ordering. A spin-flop transition was observed at Hsf=0.7T. The spin-flop field is approximately independent of pressure, although the sublattice magnetization increases with pressure. The gap and Neel temperature are presented as function is attributed to to the relative enhancement of the interdimer exchange interactions compared with the intradimer exchange interaction.Comment: 4pages,3figures To be published in J. Phys. Soc. Jpn. Vol.73 No.1