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R. J. Cava

Publications and source records attributed to R. J. Cava.

At least 253 records · Page 14Linked to original sources

Structure and magnetic properties of the Ho2Ge2O7 pyrogermanate

We report the anisotropic magnetic properties of Ho2Ge2O7 determined from dc and ac magnetization, specific heat and powder neutron diffraction experiments. The magnetic lanthanide sublattice, seen in our refinement of the tetragonal pyrogermanate crystal structure, is a right-handed spiral of edge-sharing and corner-sharing triangles; the local Ho-O coordination indicates that the crystal field is anisotropic. Susceptibility and magnetization data indeed show that the magnetism is highly anisotropic, and the magnetic structure has the Ho moments confined to the plane perpendicular to the structural spiral. The ordered moment of Ho3+, as determined from refinement of the neutron diffraction data, is 9.0 mu_B. Magnetic ordering occurs around 1.6 K. Temperature and field dependent ac susceptibility measurements show that this compound displays spin relaxation phenomena analogous to what is seen in the spin ice pyrochlore system Ho2Ti2O7.

cond-mat.other↗

Magnetothermodynamics of the Ising Antiferromagnet Dy2Ge2O7

We report systematic low temperature measurements of the DC magnetization, AC susceptibility, and heat capacity of dysprosium pyrogermanate (Dy2Ge2O7) single crystal and powder samples. Our results confirm that Dy2Ge2O7 is an anisotropic antiferromagnet. The isothermal field dependent magnetization and the integrated magnetic entropy both indicate that the Dy3+ ions behave as Ising-like spins, analogous to those in the pyrochlore spin ice materials. Both single-spin and collective spin relaxation phenomena appear to lead to spin freezing in this material, again in analogy to observations in the spin ice materials, suggesting that such phenomena may be generic to a broader class of magnetic materials.

cond-mat.str-el↗

A Ni-based Superconductor: the Heusler Compound ZrNi$_2$Ga

This work reports on the novel Heusler superconductor ZrNi2Ga. Compared to other nickel-based superconductors with Heusler structure, ZrNi2Ga exhibits a relatively high superconducting transition temperature of Tc=2.9 K and an upper critical field of 1.5 T. Electronic structure calculations show that this relatively high transition temperature is caused by a van Hove singularity, which leads to an enhanced density of states at the Fermi energy. The van Hove singularity originates from a higher order valence instability at the L-point in the electronic structure. The enhanced density of states at the Fermi level was confirmed by specific heat and susceptibility measurements. Although many Heusler compounds are ferromagnetic, our measurements of ZrNi2Ga indicate a paramagnetic state above Tc and could not reveal any traces of magnetic order down to temperatures of at least 0.35 K. We investigated in detail the superconducting state with specific heat, magnetization, and resistivity measurements. The resulting data show the typical behavior of a conventional, weakly coupled BCS (s-wave) superconductor.

cond-mat.supr-con↗

Tuning the Charge Density Wave and Superconductivity in CuxTaS2

We report the characterization of layered, 2H-type CuxTaS2, for x between 0 and 0.12. The charge density wave (CDW), at 70 K for TaS2, is destabilized with Cu doping. The sub-1K superconducting transition in undoped 2H-TaS2 jumps quickly to 2.5 K at low x, increases to 4.5 K at the optimal composition Cu0.04TaS2, and then decreases at higher x. The electronic contribution to the specific heat, first increasing and then decreasing as a function of Cu content, is 12 mJ mol-1 K-2 at Cu0.04TaS2. Electron diffraction studies show that the CDW remains present at the optimal superconducting composition, but with both a changed q vector and decreased coherence length. We present an electronic phase diagram for the system.

cond-mat.supr-con↗

Structural Disorder, Octahedral Coordination, and 2-Dimensional Ferromagnetism in Anhydrous Alums

The crystal structures of the triangular lattice, layered anhydrous alums KCr(SO4)2, RbCr(SO4)2 and KAl(SO4)2 are characterized by X-ray and neutron powder diffraction at temperatures between 1.4 and 773 K. The compounds all crystallize in the space group P-3, with octahedral coordination of the trivalent cations. In all cases, small amounts of disorder in the stacking of the triangular layers of corner sharing MO6 octahedra and SO4 tetrahedra is seen, with the MO6-SO4 network rotated in opposite directions between layers. The electron diffraction study of KCr(SO4)2 supports this model, which on average can be taken to imply trigonal prismatic coordination for the M3+ ions; as was previously reported for the prototype anhydrous alum KAl(SO4)2. The temperature dependent magnetic susceptibilities for ACr(SO4)2 (A = K,Rb,Cs) indicate the presence of predominantly ferromagnetic interactions. Low temperature powder neutron diffraction reveals that the magnetic ordering is ferromagnetic in-plane, with antiferromagnetic ordering between planes below 3 K.

cond-mat.mtrl-sci↗

Intrinsic Properties of Stoichiometric LaOFeP

DC and ac magnetization, resistivity, specific heat, and neutron diffraction data reveal that stoichiometric LaOFeP is metallic and non-superconducting above T = 0.35 K, with gamma = 12.5 mJ/mol*K. Neutron diffraction data at room temperature and T = 10 K are well described by the stoichiometric, tetragonal ZrCuSiAs structure and show no signs of structural distortions or long range magnetic ordering, to an estimated detectability limit of 0.07 uB/Fe. We propose a model, based on the shape of the iron-pnictide tetrahedron, that explains the differences between LaOFeP and LaOFeAs, the parent compound of the recently discovered high-Tc oxyarsenides, which, in contrast, shows both structural and spin density wave (SDW) transitions.

cond-mat.supr-con↗

Frustrated Ferroelectricity in Niobate Pyrochlores

The crystal structures of the A2B2O7-x Niobium-based pyrochlores Y2(Nb0.86Y0.14)2O6.91, CaYNb2O7, and Y2NbTiO7 are reported, determined by powder neutron diffraction. These compounds represent the first observation of B-site displacements in the pyrochlore structure: the B-site ions are found to be displaced from the ideal pyrochlore positions, creating electric dipoles. The orientations of these dipoles are fully analogous to orientations of the magnetic moments in Ising spin based magnetically frustrated pyrochlores. Diffuse scattering in electron diffraction patterns shows that the displacements are only short range ordered, indicative of geometric frustration of the collective dielectric state of the materials. Comparison to the crystal structure of the Nb5+ (d0) pyrochlore La2ScNbO7 supports the prediction that charge singlets, driven by the tendency of Nb to form metal-metal bonds, are present in these pyrochlores. The observed lack of long-range order to these singlets suggests that Nb4+-based pyrochlores represent the dielectric analogy to the geometric frustration of magnetic moments observed in rare earth pyrochlores.

cond-mat.str-el↗

Physical properties of the new Uranium ternary compounds U3Bi4M3 (M=Ni, Rh)

We report the properties of two new isostructural compounds, U3Bi4Ni3 and U3Bi4Rh3. The first of these compounds is non-metallic, and the second is a nearly ferromagnetic metal, both as anticipated from their electron count relative to other U-based members of the larger 3-4-3 family. For U3Bi4Rh3, a logarithmic increase of C/T below 3 K, a resistivity proportional to T^4/3, and the recovery of Fermi-liquid behavior in both properties with applied fields greater than 3T, suggest that U3Bi4Rh3 may be a new example of a material displaying ferromagnetic quantum criticality.

cond-mat.mtrl-sci↗

Structural and Magnetic Properties of Pyrochlore Solid Solutions (Y,Lu)2Ti2-x(Nb,Ta)xO7+/-y

The synthesis and characterization of the pyrochlore solid solutions, Y2Ti2-xNbxO7-y, Lu2Ti2-xNbxO7-y, Y2Ti2-xTaxO7-y and Lu2TiTaO7-y (-0.4<y<0.5), is described. Synthesis at 1600 C, and 10-5 Torr yields oxygen deficiency in all systems. All compounds are found to be paramagnetic and semiconducting, with the size of the local moments being less, in some cases substantially less, than the expected value for the number of nominally unpaired electrons present. Thermogravimetric analysis (TGA) shows that all compounds can be fully oxidized while retaining the pyrochlore structure, yielding oxygen rich pyrochlores as white powders. Powder neutron diffraction of Y2TiNbO7-based samples was done. Refinement of the data for oxygen deficient Y2TiNbO6.76 indicates the presence of a distribution of oxygen over the 8b and 48f sites. Refinement of the data for oxygen rich Y2TiNbO7.5 shows these sites to be completely filled, with an additional half filling of the 8a site. The magnetic and TGA data strongly suggest a preference for a Ti3+/(Nb,Ta)5+ combination, as opposed to Ti4+/(Nb,Ta)4+, in this pyrochlore family. In addition, the evidence clearly points to Ti3+ as the source of the localized moments, with no evidence for localized Nb4+ moments.

cond-mat.mtrl-sci↗

Magnetothermal study of Dy Stuffed Spin Ice: Dy2(DyxTi2-x)O7-x/2

We have studied the thermodynamics of the stuffed spin ice material, Dy2(DyxTi2-x)O7-x/2, in which additional Dy3+ replace Ti4+ in the pyrochlore Dy2Ti2O7. Heat capacity measurements indicate that these materials lose the spin ice zero point entropy for x >= 0.3, sharply contrasting with results on the analogous Ho materials. A finite ac susceptibility is observed as T ~ 0 in both the Ho and Dy materials with x = 0.67, which suggests that spin fluctuations persist down to T ~ 0. We propose that both the entropy and susceptibility data may be explained as a result of domains of local pyrochlore type structural order in these materials.

cond-mat.str-el↗

Intersite 4p-3d hybridization in cobalt oxides: a resonant x-ray emission spectroscopy study

We report on strong dipole transitions to 3d orbitals of neighboring Co atoms in the Co 1s x-ray absorption pre-edge. They are revealed by applying high-resolution resonant x-ray emission spectroscopy (RXES) to compounds containing CoO6 clusters. When contrasted to quadrupole local 1s3d excitations, these non-local 1s3d transitions are identified by their energy dispersion and angular dependence, their sensitivity to second-shell effects (i.e. the connection mode of the CoO6 octahedra and the bond lengths), and an upwards energy shift of 2.5 eV due to the poorer screening of the core hole. The experiment reveals that the intensity of the non-local transitions gauges the oxygen-mediated 4p-O-3d intersite hybridization. We propose a revised interpretation of the pre-edges of transition metal compounds. Detailed analysis of these new features in the pre-edge offers a unique insight in the oxygen mediated metal-metal interactions in transition metal-based systems, which is a crucial aspect in orbital ordering and related electronic and magnetic properties. In addition, the exceptional resolving power of the present 1s2p RXES experiment allows us to demonstrate the coherent second-order nature of the underlying scattering process.

cond-mat.str-el↗

Physical properties of the noncentrosymmetric superconductor Mg_10Ir_19B_16

Specific heat, electrical resistivity, and magnetic susceptibility measurements on a high quality sample of Mg10Ir19B16 provide a self-consistent determination of its superconducting properties. They indicate that Mg10Ir19B16 is a type-II superconductor (Tc=4.45K, k(0)=20), with an electron-phonon coupling constant l_ep=0.66. An analysis of the T-dependent specific heat shows that superconducting properties are dominated by an s-wave gap (D=0.7 meV). Point contact tunneling data provide evidence for multiple superconducting gaps, as expected from strong asymmetric spin-orbit coupling.

cond-mat.supr-con↗

Quantum and classical mode softening near the charge-density-wave/superconductor transition of Cu$_{x}$TiSe$_{2}$: Raman spectroscopic studies

Temperature- and x-dependent Raman scattering studies of the charge density wave (CDW) amplitude modes in CuxTiSe2 show that the amplitude mode frequency omega_o exhibits identical power-law scaling with the reduced temperature, T/T_CDW, and the reduced Cu content, x/x_c, i.e., omega_o ~ (1 - p)^0.15 for p = T/T_CDW or x/x_c, suggesting that mode softening is independent of the control parameter used to approach the CDW transition. We provide evidence that x-dependent mode softening in CuxTiSe2 is caused by the reduction of the electron-phonon coupling constant lambda due to expansion of the lattice, and that x-dependent `quantum' (T ~ 0) mode softening reveals a quantum critical point within the superconductor phase of CuxTiSe2.

cond-mat.str-el↗

Pressure effects in the triangular layered cobaltites NaxCoO2

We have measured transport properties as a function of temperature and pressure up to 30GPa in the NaxCoO2 system. For the x=0.5 sample the transition temperature at 53K increases with pressure, while paradoxically the sample passes from an insulating to a metallic ground state. A similar transition is observed in the x=0.31 sample under pressure. Compression on the x=0.75 sample transforms the sample from a metallic to an insulating state. We discuss our results in terms of interactions between band structure effects and Na+ order.

cond-mat.str-el↗

Magnetism and structure of LixCoO2 and comparison to NaxCoO2

The magnetic properties and structure of LixCoO2 for x between 0.5 and 1.0 are reported. Co4+ is found to be high-spin in LixCoO2 for x between 0.94 and 1.0 and low-spin for x between 0.50 and 0.78. Weak antiferromagnetic coupling is observed, increasing in strength as more Co4+ is introduced. At an x value of about 0.65, the temperature-independent contribution to the magnetic susceptibility and the electronic contribution to the specific heat are largest. Neutron diffraction analysis reveals that the lithium oxide layer expands perpendicular to the basal plane and the Li ions displace from their ideal octahedral sites with decreasing x. A comparison of the structures of the NaxCoO2 and LixCoO2 systems reveals that the CoO2 layer changes substantially with alkali content in the former but is relatively rigid in the latter. Further, the CoO6 octahedra in LixCoO2 are less distorted than those in NaxCoO2. We postulate that these structural differences strongly influence the physical properties in the two systems.

cond-mat.str-el↗

Crystal Structure and Physical Properties of Mg6Cu16Si7-type M6Ni16Si7, for M = Mg, Sc, Ti, Nb, and Ta

Five compounds were investigated for magnetic character and superconductivity, all with non-magnetic nickel and band structures containing flat bands and steep bands. The syntheses and crystal structures, refined by powder X-ray diffraction, are reported for M6Ni16Si7, where M = Mg, Sc, Ti, Nb, and Ta. All compounds form in the Mg6Cu16Si7 structure type. Resistance measurements are also reported on M6Ni16Si7 (M = Mg, Sc, Ti, and Nb) down to 0.3 K, with all four showing metallic conductivity. No superconductivity is observed. Magnetization measurements for all compounds reveal essentially temperature independent paramagnetism, with a tendency toward more enhanced low temperature paramagnetism for the cases of Mg6Ni16Si7 and Sc6Ni16Si7.

cond-mat.supr-con↗

The anomalous Hall Effect and magnetoresistance in the layered ferromagnet Fe_{1/4}TaS_2: the inelastic regime

The large magnetic anisotropy in the layered ferromagnet Fe_{1/4}TaS_2 leads to very sharp reversals of the magnetization $\bf M$ at the coercive field. We have exploited this feature to measure the anomalous Hall effect (AHE), focussing on the AHE conductivity $σ^A_{xy}$ in the inelastic regime. At low temperature T (5-50 K), $σ^A_{xy}$ is T-independent, consistent with the Berry-phase/Karplus-Luttinger theory. Above 50 K, we extract an inelastic AHE conductivity $σ^{in}_{xy}$ that scales as the square of $Δρ$ (the T dependent part of the resistivity $ρ$). The term $σ^{in}_{xy}$ clarifies the T dependence and sign-reversal of the AHE coefficient R_s(T). We discuss the possible ubiquity of $σ^{in}_{xy}$ in ferromagnets, and ideas for interpreting its scaling with $(Δρ)^2$. Measurements of the magnetoresistance (MR) reveal a rich pattern of behavior vs. T and field tilt-angle. We show that the 2 mechanisms, the anisotropic MR effect and field-suppression of magnons, account for the intricate MR behavior, including the bow-tie features caused by the sharp reversals in $\bf M$.

cond-mat.str-el↗

Structures of the reduced niobium oxides Nb12O29 and Nb22O54

The crystal structure of Nb22O54 is reported for the first time, and the structure of orthorhombic Nb12O29 is reexamined, resolving previous ambiguities. Single crystal x-ray and electron diffraction were employed. These compounds were found to crystallize in the space groups P2/m (a = 15.7491(2) A, b = 3.8236(3) A, c = 17.8521(2) A, beta = 102.029(3)) and Cmcm (a = 3.8320(2) A, b = 20.7400(9) A, c = 28.8901(13) A) respectively and share a common structural unit, a 4x3 block of corner sharing NbO6 octahedra. Despite different constraints imposed by symmetry these blocks are very similar in both compounds. Within a block, it is found that the niobium atoms are not located in the centers of the oxygen octahedra, but rather are displaced inward toward the center of the block forming an apparent antiferroelectric state. Bond valence sums and bond lengths do not show the presence of charge ordering, suggesting that all 4d electrons are delocalized in these compounds at the temperature studied, T = 200 K.

cond-mat.mtrl-sci↗