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T. M. McQueen

Publications and source records attributed to T. M. McQueen.

64 records · Page 4Linked to original sources

Superconductivity at 2.2K in La3Ni4P4O2

We report the observation of superconductivity in La3Ni4P4O2 at 2.2 K. The layer stacking in this compound results in an asymmetric distribution of charge reservoir layers around the Ni2P2 planes. The estimated Wilson ratio, Rw ~ 5, indicates the presence of a strongly enhanced normal state susceptibility, but many of the basic superconducting characteristics are conventional. The estimated electronic contribution to the specific heat, gamma ~ 6.2 mJ mol-Ni^-1K^-2, is about 2/3 of that found in layered nickel borocarbide superconductors.

cond-mat.supr-con↗

Extreme Sensitivity of Superconductivity to Stoichiometry in FeSe (Fe1+dSe)

The recently discovered iron arsenide superconductors, which display superconducting transition temperatures as high as 55 K, appear to share a number of general features with high-Tc cuprates, including proximity to a magnetically ordered state and robustness of the superconductivity in the presence of disorder. Here we show that superconductivity in Fe1+dSe, the parent compound of the superconducting arsenide family, is destroyed by very small changes in stoichiometry. Further, we show that non-superconducting Fe1+dSe is not magnetically ordered down to low temperatures. These results suggest that robust superconductivity and immediate instability against an ordered magnetic state should not be considered as intrinsic characteristics of iron-based superconducting systems, and that Fe1+dSe may present a unique opportunity for determining which materials characteristics are critical to the existence of superconductivity in high Tc iron arsenide superconductors and which are not.

cond-mat.supr-con↗

Origin and tuning of the magnetocaloric effect for the magnetic refrigerant MnFe(P1-xGex)

Neutron diffraction and magnetization measurements of the magneto refrigerant Mn1+yFe1-yP1-xGex reveal that the ferromagnetic and paramagnetic phases correspond to two very distinct crystal structures, with the magnetic entropy change as a function of magnetic field or temperature being directly controlled by the phase fraction of this first-order transition. By tuning the physical properties of this system we have achieved a maximum magnetic entropy change exceeding 74 J/Kg K for both increasing and decreasing field, more than twice the value of the previous record.

cond-mat.mtrl-sci↗

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↗

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↗

Magnetic Structure and Properties of the S = 5/2 Triangular Antiferromagnet $α$-NaFeO$_2$

The magnetic properties of $α$-NaFeO$_2$ are studied by neutron diffraction and magnetization measurements. An ordered phase with spins aligned along the b$_hex$ axis exists at low temperatures (T < 4 K). At intermediate temperatures (4 K < T < 11 K), the system passes through an incommensurate ordered phase before transforming into a short range ordered state at higher temperatures that persists up to at least 50 K. Although the short range ordering does not persist to room temperature according to neutron diffraction, the magnetic susceptibility does not follow Curie-Weiss behavior, even up to 320 K. This rich magnetic behavior can be understood qualitatively as a competition between different magnetic exchange interactions that are similar in magnitude. The delicate balance between these interactions makes $α$-NaFeO$_2$ a candidate for more detailed theoretical work to understand magnetic behavior in frustrated magnetic systems.

cond-mat.str-el↗

Stuffed Rare Earth Pyrochlore Solid Solutions

Synthesis and crystal structures are described for the compounds Ln2(Ti2-xLnx)O7-x/2, where Ln = Tb, Dy, Ho, Er, Tm, Yb, Lu, and x ranges from 0 to 0.67. Rietveld refinements on X-ray powder diffraction data indicate that in Tb and Dy titanate pyrochlores, extra Ln3+ cations mix mainly on the Ti4+ site with little disorder on the original Ln3+ site. For the smaller rare earths (Ho-Lu), stuffing additional lanthanide ions results in a pyrochlore to defect fluorite transition, where the Ln3+ and Ti4+ ions become completely randomized at the maximum (x=0.67). In all of these Ln-Ti-O pyrochlores, the addition of magnetic Ln3+ in place of nonmagnetic Ti4+ adds edge sharing tetrahedral spin interactions to a normally corner sharing tetrahedral network of spins. The increase in spin connectivity in this family of solid solutions represents a new avenue for investigating geometrical magnetic frustration in the rare earth titanate pyrochlores.

cond-mat.str-el↗