Anisotropic optical response of the mixed-valent Mott-Hubbard insulator NaCu2O2

We report the results of a comprehensive spectroscopic ellipsometry study of NaCu2O2, a compound composed of chains of edge-sharing Cu2+O4 plaquettes and planes of Cu1+ ions in a O-Cu1+-O dumbbell configuration, in the spectral range 0.75-6.5 eV at temperatures 7 -300 K. The spectra of the dielectric function for light polarized parallel to the Cu1+ planes reveal a strong in-plane anisotropy of the interband excitations. Strong and sharp absorption bands peaked at 3.45 eV (3.7 eV) dominate the spectra for polarization along (perpendicular) to the Cu2+O2 chains. They are superimposed on flat and featureless plateaux above the absorption edges at 2.25 eV (2.5 eV). Based on density-functional calculations, the anomalous absorption peaks can be assigned to transitions between bands formed by Cu1+ 3dxz(dyz) and Cu2+ 3dxy orbitals, strongly hybridized with O pstates. The major contribution to the background response comes from transitions between Cu1+ 3dz2 and 4px(py) bands. This assignment accounts for the measured in-plane anisotropy. The dielectric response along the Cu2+O2 chains develops a weak two-peak structure centered at 2.1 and 2.65 eV upon cooling below 100 K, along with the appearance of spin correlations along the Cu2+O2 chains. These features bear a striking resemblance to those observed in the single-valent Cu2+O2 chain compound LiCuVO4, which were identified as an exciton doublet associated with transitions to the upper Hubbard band that emerges as a consequence of the long-range Coulomb interaction between electrons on neighboring Cu2+ sites along the chains. An analysis of the spectral weights of these features yields the parameters characterizing the on-site and long-range Coulomb interactions.Comment: 12 pages, 12 figure

Magnetic structure of the edge-sharing copper oxide chain compound NaCu2O2

Single-crystal neutron diffraction has been used to determine the incommensurate magnetic structure of NaCu2O2, a compound built up of chains of edge-sharing CuO4 plaquettes. Magnetic structures compatible with the lattice symmetry were identified by a group-theoretical analysis, and their magnetic structure factors were compared to the experimentally observed Bragg intensities. In conjunction with other experimental data, this analysis yields an elliptical helix structure in which both the helicity and the polarization plane alternate among copper-oxide chains. This magnetic ground state is discussed in the context of the recently reported multiferroic properties of other copper-oxide chain compounds

Magnetic phase diagram of Sr3Fe2O7−xSr_3 Fe_2 O_{7-x}

Magnetometry, electrical transport, and neutron scattering measurements were performed on single crystals of the Fe^{4+}-containing perovskite-related phase Sr_3Fe_2O_7-x as a function of oxygen content. Although both the crystal structure and electron configuration of this compound are closely similar to those of well-studied ruthenates and manganates, it exhibits very different physical properties. The fully-oxygenated compound (x=0) exhibits a charge-disproportionation transition at T_D = 340 K, and an antiferromagnetic transition at T_N = 115 K. For temperatures T \leq T_D, the material is a small-gap insulator; the antiferromagnetic order is incommensurate, which implies competing exchange interactions between the Fe^{4+} moments. The fully-deoxygenated compound (x=1) is highly insulating, and its Fe^{3+} moments exhibit commensurate antiferromagnetic order below T_N ~ 600 K. Compounds with intermediate x exhibit different order with lower T_N, likely as a consequence of frustrated exchange interactions between Fe^{3+} and Fe^{4+} sublattices. A previous proposal that the magnetic transition temperature reaches zero is not supported.Comment: 8 pages, 6 figure

Magnetic excitations and phonons in the spin-chain compound NaCu2O2

We report an inelastic light scattering study of single-crystalline NaCu$_2$O$_2$, a spin-chain compound known to exhibit a phase with helical magnetic order at low temperatures. Phonon excitations were studied as a function of temperature and light polarization, and the phonon frequencies are compared to the results of ab-initio lattice dynamical calculations, which are also reported here. The good agreement between the observed and calculated modes allows an assignment of the phonon eigenvectors. Two distinct high-energy two-magnon features as well as a sharp low-energy one-magnon peak were also observed. These features are discussed in terms of the magnon modes expected in a helically ordered state. Their polarization dependence provides evidence of substantial exchange interactions between two closely spaced spin chains within a unit cell. At high temperatures, the spectral features attributable to magnetic excitations are replaced by a broad, quasielastic mode due to overdamped spin excitations

Spin liquid in a single crystal of the frustrated diamond lattice antiferromagnet CoAl2O4

We study spin liquid in the frustrated diamond lattice antiferromagnet CoAl2O4 by means of single crystal neutron scattering in zero and applied magnetic field. The magnetically ordered phase appearing below TN=8 K remains nonconventional down to 1.5 K. The magnetic Bragg peaks at the q=0 positions remain broad and their profiles have strong Lorentzian contribution. Additionally, they are connected by weak diffuse streaks along the directions. These observations are explained within the spiral spin liquid model as short-range magnetic correlations of spirals populated at these finite temperatures, as the energy minimum around q=0 is flat and the energy of excited states with q=(111) is low. The agreement is only qualitative, leading us to suspect that microstructure effects are also important. Magnetic field significantly perturbs spin correlations. The 1.5 K static magnetic moment increases from 1.58 mB/Co at zero field to 2.08 mB/Co at 10 T, while the magnetic peaks, being still broad, acquire almost Gaussian profile. Spin excitations are rather conventional spin waves at zero field, resulting in the exchange parameters J1=0.92(1) meV, J2=0.101(2) meV and the anisotropy term D=-0.0089(2) meV for CoAl2O4. The application of a magnetic field leads to a pronounced broadening of the excitations at the zone center, which at 10 T appear gapless and nearly featureless

Magnetoresistance Effects in SrFeO(3-x): Dependence on Phase Composition and Relation to Magnetic and Charge Order

Single crystals of iron(IV) rich oxides SrFeO(3-x) with controlled oxygen content have been studied by Moessbauer spectroscopy, magnetometry, magnetotransport measurements, Raman spectroscopy, and infrared ellipsometry in order to relate the large magnetoresistance (MR) effects in this system to phase composition, magnetic and charge order. It is shown that three different types of MR effects occur. In cubic SrFeO3 (x = 0) a large negative MR of 25% at 9 T is associated with a hitherto unknown 60 K magnetic transition and a subsequent drop in resistivity. The 60 K transition appears in addition to the onset of helical ordering at ~130 K. In crystals with vacancy-ordered tetragonal SrFeO(3-x) as majority phase (x ~0.15) a coincident charge/antiferromagnetic ordering transition near 70 K gives rise to a negative giant MR effect of 90% at 9 T. A positive MR effect is observed in tetragonal and orthorhombic materials with increased oxygen deficiency (x = 0.19, 0.23) which are insulating at low temperatures. Phase mixtures can result in a complex superposition of these different MR phenomena. The MR effects in SrFeO(3-x) differ from those in manganites as no ferromagnetic states are involved

Disparity of superconducting and pseudogap scales in low-Tc Bi-2201 cuprates

We experimentally study transport and intrinsic tunneling characteristics of a single-layer cuprate Bi(2+x)Sr(2-y)CuO(6+delta) with a low superconducting critical temperature Tc < 4 K. It is observed that the superconducting energy, critical field and fluctuation temperature range are scaling down with Tc, while the corresponding pseudogap characteristics have the same order of magnitude as for high-Tc cuprates with 20 to 30 times higher Tc. The observed disparity of the superconducting and pseudogap scales clearly reveals their different origins.Comment: 5 page