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R J Cava

Publications and source records attributed to R J Cava.

At least 19 recordsLinked to original sources

Complete d-band dispersion relation in sodium cobaltates.

We utilize fine-tuned polarization selection coupled with excitation-energy variation of photoelectron signal to image the complete d-band dispersion relation in sodium cobaltates. A hybridization gap anticrossing is observed along the Brillouin zone corner and the full quasiparticle band is found to emerge as a many-body entity lacking a pure orbital polarization. At low dopings, the quasiparticle bandwidth (Fermion scale, many-body E(F) approximately 0.25 eV) is found to be smaller than most known oxide metals. The low-lying density of states is found to be in agreement with bulk-sensitive thermodynamic measurements for nonmagnetic dopings where the 2D Luttinger theorem is also observed to be satisfied.

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Unconventional dynamics in triangular Heisenberg antiferromagnet NaCrO2.

We report magnetization, specific heat, muon spin rotation, and Na NMR measurements on the S=3/2 rhombohedrally stacked Heisenberg antiferromagnet NaCrO2. This compound appears to be a good candidate for the study of isotropic triangular Heisenberg antiferromagnets with very weak interlayer coupling. While specific heat and magnetization measurements indicate the onset of a transition in the range Tc approximately 40-50 K, both muon spin rotation and NMR reveal a fluctuating crossover regime extending well below Tc, with a peak of relaxation rate T1(-1) around T approximately 25 K. This novel finding is discussed within the context of excitations in the triangular Heisenberg antiferromagnets.

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Orbitally driven spin-singlet dimerization in S=1 La4Ru2O10.

Using x-ray absorption spectroscopy at the Ru-L2,3 edge we reveal that the Ru4+ ions remain in the S=1 spin state across the rare 4d-orbital ordering transition and spin-gap formation. We find using local spin density approximation + Hubbard U band structure calculations that the crystal fields in the low-temperature phase are not strong enough to stabilize the S=0 state. Instead, we identify a distinct orbital ordering with a significant anisotropy of the antiferromagnetic exchange couplings. We conclude that La4Ru2O10 appears to be a novel material in which the orbital physics drives the formation of spin-singlet dimers in a quasi-two-dimensional S=1 system.

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Large enhancement of the thermopower in Na(x)CoO2 at high Na doping.

Research on the oxide perovskites has uncovered electronic properties that are strikingly enhanced compared with those in conventional metals. Examples are the high critical temperatures of the cuprate superconductors and the colossal magnetoresistance in the manganites. The conducting layered cobaltate Na(x)CoO2 exhibits several interesting electronic phases as the Na content x is varied, including water-induced superconductivity and an insulating state that is destroyed by field. Initial measurements showed that, in the as-grown composition, Na(x)CoO2 has moderately large thermopower S and conductivity sigma. However, the prospects for thermoelectric cooling applications faded when the figure of merit Z was found to be small at this composition (0.6 0.75, S undergoes an even steeper enhancement. At the critical doping x(p) approximately 0.85, Z (at 80 K) reaches values approximately 40 times larger than in the as-grown crystals. We discuss prospects for low-temperature thermoelectric applications.

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Low-lying quasiparticle states and hidden collective charge instabilities in parent cobaltate superconductors.

We report a state-of-the-art photoemission (angle-resolved photoemission spectroscopy) study of high quality single crystals of NaxCoO2 the series focusing on the fine details of the low-energy states. The Fermi velocity is found to be small (<0.5 eV A) and only weakly anisotropic over the Fermi surface at all dopings, setting the size of the pair wave function to be on the order of 10-20 nm. In the low-doping regime, the exchange interlayer splitting vanishes and two-dimensional collective instabilities such as 120 degrees -type fluctuations become kinematically allowed. Our results suggest that the unusually small Fermi velocity and the unique symmetry of kinematic instabilities distinguish cobaltates from most other oxide superconductors.

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Quasiparticle dynamics in the vicinity of metal-insulator phase transition in NaxCoO2.

Layered cobaltates embody novel realizations of correlated matter on a spin-1/2 triangular lattice. We report a high-resolution systematic photoemission study of the insulating cobaltates. The observation of a single-particle gap opening and band folding provides direct evidence of anisotropic particle-hole instability on the Fermi surface due to its unique topology. Overlap of the measured Fermi surface is observed with the square root 3xsquare root 3 charge-order Brillouin zone near x=1/3 but not at x=1/2 where the insulating transition is actually observed. Unlike conventional density waves, charge stripes, or band insulators, the onset of the gap depends on the quasiparticle's quantum coherence which is found to occur well below the disorder-order symmetry breaking temperature of the crystal (the first known example of its kind).

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Slow spin relaxation in a highly polarized cooperative paramagnet.

We report measurements of the ac susceptibility of the cooperative paramagnet Tb2Ti2O7 in a strong magnetic field. Our data show the expected saturation maximum in chi(T) and also an unexpected frequency dependence of this peak at low frequencies (<1 Hz), suggesting very slow spin relaxations are occurring. Measurements on samples diluted with nonmagnetic Y3+ or Lu3+ and complementary measurements on pure and diluted Dy2Ti2O7 strongly suggest that the relaxation is associated with dipolar spin correlations, representing unusual cooperative behavior in a paramagnetic system.

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Contemporary superconducting materials.

Superconductors currently under active study are briefly described from a chemical perspective. The author's current views on those superconductors, the role of theory in searching for new superconductors, and possibilities for new superconducting materials that might be found in the future are presented.

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Magnetically driven ferroelectric order in Ni3V2O8.

We show that long-range ferroelectric and incommensurate magnetic order appear simultaneously in a single phase transition in Ni3V2O8. The temperature and magnetic-field dependence of the spontaneous polarization show a strong coupling between magnetic and ferroelectric orders. We determine the magnetic symmetry using Landau theory for continuous phase transitions, which shows that the spin structure alone can break spatial inversion symmetry leading to ferroelectric order. This phenomenological theory explains our experimental observation that the spontaneous polarization is restricted to lie along the crystal b axis and predicts that the magnitude should be proportional to a magnetic order parameter.

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Orbital dependence of the fermi liquid state in Sr2RuO4.

We have used angle-resolved photoemission spectroscopy to determine the bulk electronic structure of Sr(2)RuO(4) above and below the Fermi liquid crossover near 25 K. Our measurements indicate that the properties of the system are highly orbital dependent. The quasi-2D gamma band displays Fermi liquid behavior while the remaining low energy bands show exotic properties consistent with quasi-1D behavior. In the Fermi liquid state below 25 K, the gamma band dominates the electronic properties, while at higher temperatures the quasi-1D beta and alpha bands become more important.

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Competing magnetic phases on a kagomé staircase.

We present thermodynamic and neutron data on Ni3V2O8, a spin-1 system on a kagomé staircase. The extreme degeneracy of the kagomé antiferromagnet is lifted to produce two incommensurate phases at finite T--one amplitude modulated, the other helical--plus a commensurate canted antiferromagnet for T-->0. The H-T phase diagram is described by a model of competing first and second neighbor interactions with smaller anisotropic terms. Ni3V2O8 thus provides an elegant example of order from subleading interactions in a highly frustrated system.

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Anomalous hall heat current and nernst effect in the CuCr2Se4-xBrx ferromagnet.

In a ferromagnet, an anomalous Hall heat current, given by the off-diagonal Peltier term alpha(xy), accompanies the anomalous Hall current. By combining Nernst, thermopower, and Hall experiments, we have measured how alpha(xy) varies with hole density and lifetime tau in CuCr2Se4-xBrx. At low temperatures T, we find that alpha(xy) is independent of tau, consistent with anomalous-velocity theories. Its magnitude is fixed by a microscopic geometric area A approximately 34 A(2). Our results are incompatible with some models of the Nernst effect in ferromagnets.

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Schizophrenic electrons in ruthenium-based oxides.

Ruthenium and oxygen form many ternary compounds in which the Ru 4d states and O 2p states are strongly hybridized. In some such compounds, this hybridization leads to the loss of local magnetic moment character for the Ru, and in others it does not. The factors that determine which is the case are often subtle and poorly understood. The richness of structure types seen in ternary Ru oxides leads to a corresponding richness in electronic and magnetic properties. This article briefly describes the author's current views on these materials.

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Fermi surface and quasiparticle dynamics of Na0.7CoO2 investigated by angle-resolved photoemission spectroscopy.

We present the first angle-resolved photoemission study of Na0.7CoO2, the host material of the superconducting NaxCoO2.nH(2)O series. Our results show a hole-type Fermi surface, a strongly renormalized quasiparticle band, a small Fermi velocity, and a large Hubbard U. The quasiparticle band crosses the Fermi level from M toward Gamma suggesting a negative sign of effective single-particle hopping t(eff) (about 10 meV) which is on the order of magnetic exchange coupling J in this system. Quasiparticles are well defined only in the T-linear resistivity (non-Fermi-liquid) regime. Unusually small single-particle hopping and unconventional quasiparticle dynamics may have implications for understanding the phase of matter realized in this new class of a strongly interacting quantum system.

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Charge ordering, commensurability, and metallicity in the phase diagram of the layered NaxCoO2.

The phase diagram of nonhydrated NaxCoO2 has been determined by changing the Na content x using a series of chemical reactions. As x increases from 0.3, the ground state goes from a paramagnetic metal to a charge-ordered insulator (at x=1/2), then to a "Curie-Weiss metal" (around 0.70), and finally to a weak-moment magnetically ordered state (x>0.75). The unusual properties of the state at 1/2 (including particle-hole symmetry at low T and enhanced thermal conductivity) are described. The strong coupling between the Na ions and the holes is emphasized.

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Dissipationless anomalous Hall current in the ferromagnetic spinel CuCr2Se4-xBrx.

In a ferromagnet, an applied electric field E invariably produces an anomalous Hall current JH that flows perpendicular to the plane defined by E and M (the magnetization). For decades, the question of whether JH is dissipationless (independent of the scattering rate) has been debated without experimental resolution. In the ferromagnetic spinel CuCr2Se4-xBrx, the resistivity rho (at low temperature) may be increased by several decades by varying x (Br) without degrading M. We show that JH/E (normalized per carrier, at 5 kelvin) remains unchanged throughout. In addition to confirming the dissipationless nature of JH, our finding has implications for the generation and study of spin-Hall currents in bulk samples.

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Potential signature of a Kosterlitz-Thouless transition in BaNi2V2O8.

ESR measurements are reported for the quasi-two-dimensional honeycomb antiferromagnet BaNi2V2O8. Planar anisotropic properties are confirmed by angular dependent investigations of resonance field and linewidth. The divergence of the temperature-dependent linewidth on approaching T(N) from above is described in terms of the Kosterlitz-Thouless transition, the critical behavior close to long-range magnetic order, and the 2D Heisenberg antiferromagnet. We provide arguments that the Kosterlitz-Thouless scenario is compatible with the observed critical exponent and suggest BaNi2V2O8 is a weakly anisotropic 2D Heisenberg antiferromagnet.

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