A magnetic continuum in the cobalt-based honeycomb magnet BaCo2(AsO4)2.

Quantum spin liquids (QSLs) are topologically ordered states of matter that host fractionalized excitations. A particular route towards a QSL is via strongly bond-dependent interactions on the hexagonal lattice. A number of Ru- and Ir-based candidate Kitaev QSL materials have been pursued, but all have appreciable non-Kitaev interactions. Using time-domain terahertz spectroscopy, we observed a broad magnetic continuum over a wide range of temperatures and fields in the honeycomb cobalt-based magnet BaCo2(AsO4)2, which has been proposed to be a more ideal version of a Kitaev QSL. Applying an in-plane magnetic field of ~0.5 T suppresses the magnetic order, and at higher fields, applying the field gives rise to a spin-polarized state. Under a 4 T magnetic field that was oriented principally out of plane, a broad magnetic continuum was observed that may be consistent with a field-induced QSL. Our results indicate BaCo2(AsO4)2 is a promising QSL candidate.

Direct assignment of molecular vibrations via normal mode analysis of the neutron dynamic pair distribution function technique.

For over a century, vibrational spectroscopy has enhanced the study of materials. Yet, assignment of particular molecular motions to vibrational excitations has relied on indirect methods. Here, we demonstrate that applying group theoretical methods to the dynamic pair distribution function analysis of neutron scattering data provides direct access to the individual atomic displacements responsible for these excitations. Applied to the molecule-based frustrated magnet with a potential magnetic valence-bond state, LiZn2Mo3O8, this approach allows direct assignment of the constrained rotational mode of Mo3O13 clusters and internal modes of MoO6 polyhedra. We anticipate that coupling this well known data analysis technique with dynamic pair distribution function analysis will have broad application in connecting structural dynamics to physical properties in a wide range of molecular and solid state systems.

Bandwidth tuning triggers interplay of charge order and superconductivity in two-dimensional organic materials.

We observe charge-order fluctuations in the quasi-two-dimensional organic superconductor ß''-(BEDT-TTF)2SF5CH2CF2SO3, both by means of vibrational spectroscopy, locally probing the fluctuating charge order, and by investigating the in-plane dynamical response by infrared reflectance spectroscopy. The decrease of the effective electronic interaction in an isostructural metal suppresses both charge-order fluctuations and superconductivity, pointing to their interplay. We compare the results of our experiments with calculations on the extended Hubbard model.

Collective excitations in the charge-ordered phase of α-(BEDT-TTF)2I3.

The charge response of a charge-ordered state in the organic conductor α-(BEDT-TTF)2I3 is characterized by dc resistivity, dielectric and optical spectroscopy in different crystallographic directions within the two-dimensional conduction layer. Two dielectric modes are detected. The large mode is related to the phasonlike excitation of the 2k(F) bond-charge density wave which forms in the ab plane. The small dielectric mode is associated with the motion of domain-wall pairs along the a and b axes between two types of domains which are created due to inversion symmetry breaking.

Quasiparticles at the verge of localization near the Mott metal-insulator transition in a two-dimensional material.

The dynamics of charge carriers close to the Mott transition is explored theoretically and experimentally in the quasi-two-dimensional organic charge-transfer salt, kappa-(BEDT-TTF)_(2)Cu[N(CN)_(2)]Br_(x)Cl_(1-x), with varying Br content. The frequency dependence of the conductivity deviates significantly from simple Drude model behavior: there is a strong redistribution of spectral weight as the Mott transition is approached and with temperature. The effective mass of the quasiparticles increases considerably when coming close to the insulating phase. A dynamical mean-field-theory treatment of the relevant Hubbard model gives good quantitative description of experimental data.

Non-fermi liquid behavior in nearly charge ordered layered metals.

Non-Fermi liquid behavior is shown to occur in two-dimensional metals which are close to a charge ordering transition driven by the Coulomb repulsion. A linear temperature dependence of the scattering rate together with an increase of the electron effective mass occur above T*, a temperature scale much smaller than the Fermi temperature. It is shown that the anomalous temperature dependence of the optical conductivity of the quasi-two-dimensional organic metal alpha-(BEDT-TTF)2MHg(SCN)4, with M = NH4 and Rb, above T* = 50-100K, agrees qualitatively with predictions for the electronic properties of nearly charge ordered two-dimensional metals.

Proximity of the layered organic conductors alpha-(BEDT-TTF)2MHg(SCN)4 (M = K, NH4) to a charge-ordering transition.

While the optical properties of the superconducting salt alpha-(BEDT-TTF)(2)-NH4Hg(SCN)(4) remain metallic down to 2 K, in the nonsuperconducting K analog a pseudogap develops at frequencies of about 200 cm(-1) for temperatures T<200 K. We show that the optical conductivity calculated with exact-diagonalization techniques on an extended Hubbard model at quarter filling is consistent with the observed low-frequency feature. We argue that the different optical responses observed are a consequence of the proximity of these compounds to a charge-ordering transition driven by the intermolecular Coulomb repulsion.

New molecular complexes of fullerenes C60 and C70 with tetraphenylporphyrins [M(tpp)], in which M=H2, Mn, Co, Cu, Zn, and FeCl.

New molecular complexes of fullerenes C60 and C70 with tetraphenylporphyrins [M(tpp)] in which M-H2, MnII, CoII, CuII, ZnII and Fe(III)Cl, have been synthesised. Crystal structures of two C60 complexes with H2TPP, which differ only in the number of benzene solvated molecules, and C60 and C70 complexes with [Cu(tpp)] have been studied. The fullerene molecules form a honeycomb motif in H2TPP.2C60. 3C6H6, puckered graphite-like layers in H2TPP.2C60.4C6H6, zigzag chains in [Cu(tpp)].C70.1.5C7H8.0.5C2HCl3 and columns in [Cu(tpp)]2.C60. H2TPP has van der Waals contacts with C60 through nitrogen atoms and phenyl groups. Copper atoms of the [Cu(tpp)] molecules are weakly coordinated with C70, but form no shortened contacts with C60. The formation of molecular complexes with fullerenes affects the ESR spectra of [M(tpp)] (M = Mn, Co and Cu). [Mn(tpp)] in the complex with C70 lowers its spin state from S = 5/2 to S = 1/2, whereas [Co(tpp)] and [Cu(tpp)] change the constants of hyperfine interaction. ESR, IR, UV-visible and X-ray photoelectron spectroscopic data show no noticeable charge transfer from the porphyrinate to the fullerene molecules.