Tuning the spin dynamics of kagome systems

Despite the conceptional importance of realizing spin liquids in solid states only few compounds are known. On the other side the effect of lattice distortions and anisotropies on the magnetic exchange topology and the fluctuation spectrum are an interesting problem. We compare the excitation spectra of the two s=1/2 kagome lattice compounds volborthite and vesignieite using Raman scattering. We demonstrate that even small modifications of the crystal structure may have a huge effect on the phonon spectrum and low temperature properties.Comment: 3 pages, 2 figure

Relation between Kitaev magnetism and structure in α\alpha-RuCl3_3

Raman scattering has been employed to investigate lattice and magnetic excitations of the honeycomb Kitaev material $\alpha$-RuCl$_3$ and its Heisenberg counterpart CrCl$_3$. Our phonon Raman spectra give evidence for a first-order structural transition from a monoclinic to a rhombohedral structure for both compounds. Significantly, only $\alpha$-RuCl$_3$ features a large thermal hysteresis, consistent with the formation of a wide phase of coexistence. In the related temperature interval of $70-170$ K, we observe a hysteretic behavior of magnetic excitations as well. The stronger magnetic response in the rhombohedral compared to the monoclinic phase evidences a coupling between the crystallographic structure and low-energy magnetic response. Our results demonstrate that the Kitaev magnetism concomitant with fractionalized excitations is susceptible to small variations of bonding geometry.Comment: 9 pages, 8 figures, To appear in PR

Collective Singlet Excitations and Evolution of Raman Spectral Weights in the 2D Spin Dimer Compound SrCu2(BO3)2

We present a Raman light scattering study of the two-dimensional quantum spin system SrCu2(BO3)2 and show that the magnetic excitation spectrum has a rich structure, including several well-defined bound state modes at low temperature, and a scattering continuum and quasielastic light scattering contributions at high temperature. The key to the understanding of the unique features of SrCu2(BO3)2 is the presence of strong interactions between well-localized triplet excitations in the network of orthogonal spin dimers realized in this compound. Based on our analysis of the Heisenberg model relevant for this material, we argue that the collective excitations involving two and three-particle singlet bound states have large binding energies and are observed as well-defined peaks in the Raman spectrum.Comment: 5 pages, 2 figures. Revised version, to appear in Phys. Rev. Lett. (2000

Comparative investigation of the coupled-tetrahedra quantum spin systems Cu2Te2O5X2, X=Cl, Br and Cu4Te5O12Cl4

We present a comparative study of the coupled-tetrahedra quantum spin systems Cu2Te2O5X2, X=Cl, Br (Cu-2252(X)) and the newly synthesized Cu4Te5O12Cl4 (Cu-45124(Cl)) based on ab initio Density Functional Theory calculations. The magnetic behavior of Cu-45124(Cl) with a phase transition to an ordered state at a lower critical temperature T$_c$=13.6K than in Cu-2252(Cl) (T$_c$=18K) can be well understood in terms of the modified interaction paths. We identify the relevant structural changes between the two systems and discuss the hypothetical behavior of the not yet synthesized Cu-45124(Br) with an ab initio relaxed structure using Car-Parrinello Molecular Dynamics.Comment: 2 pages, 1 figure; submitted to Proceedings of M2S-HTSC VIII, Dresden 200

TiOCl, an orbital-ordered system?

We present first principles density functional calculations and downfolding studies of the electronic and magnetic properties of the layered quantum spin system TiOCl. We discuss explicitely the nature of the exchange pathes and attempt to clarify the concept of orbital ordering in this material. An analysis of the electronic structure of slightly distorted structures according to the phononic modes allowed in this material suggests that this system is subject to large orbital fluctuations driven by the electron-phonon coupling. Based on these results, we propose a microscopic explanation of the behavior of TiOCl near the phase transition to a spin-gapped system.Comment: Some figures are compressed, for higher quality please contact the author

Longitudinal magnon in the tetrahedral spin system Cu2Te2O5Br2 near quantum criticality

We present a comprehensive study of the coupled tetrahedra-compound Cu2Te2O5Br2 by theory and experiments in external magnetic fields. We report the observation of a longitudinal magnon in Raman scattering in the ordered state close to quantum criticality. We show that the excited tetrahedral-singlet sets the energy scale for the magnetic ordering temperature T_N. This energy is determined experimentally. The ordering temperature T_N has an inverse-log dependence on the coupling parameters near quantum criticality

Microscopic Evidence of Spin State Order and Spin State Phase Separation in Layered Cobaltites RBaCo2O5.5 with R=Y, Tb, Dy, and Ho

We report muon spin relaxation measurements on the magnetic structures of RBaCo_2O_5.5 with R=Y, Tb, Dy, and Ho. Three different phases, one ferrimagnetic and two antiferromagnetic, are identified below 300 K. They consist of different ordered spin state arrangements of high-, intermediate-, and low-spin Co^3+ of CoO_6 octahedra. Phase separation into well separated regions with different spin state order is observed in the antiferromagnetic phases. The unusual strongly anisotropic magnetoresistance and its onset at the FM-AFM phase boundary is explained.Comment: 4 pages, accepted for publication in Phys. Rev. Let

Enhanced quasiparticle dynamics of quantum well states: the giant Rashba system BiTeI and topological insulators

In the giant Rashba semiconductor BiTeI electronic surface scattering with Lorentzian linewidth is observed that shows a strong dependence on surface termination and surface potential shifts. A comparison with the topological insulator Bi2Se3 evidences that surface confined quantum well states are the origin of these processes. We notice an enhanced quasiparticle dynamics of these states with scattering rates that are comparable to polaronic systems in the collision dominated regime. The Eg symmetry of the Lorentzian scattering contribution is different from the chiral (RL) symmetry of the corresponding signal in the topological insulator although both systems have spin-split surface states.Comment: 6 pages, 5 figure