On the Chemistry and Physical Properties of Flux and Floating Zone Grown SmB6 Single Crystals.

Recent theoretical and experimental findings suggest the long-known but not well understood low temperature resistance plateau of SmB6 may originate from protected surface states arising from a topologically non-trivial bulk band structure having strong Kondo hybridization. Yet others have ascribed this feature to impurities, vacancies, and surface reconstructions. Given the typical methods used to prepare SmB6 single crystals, flux and floating-zone procedures, such ascriptions should not be taken lightly. We demonstrate how compositional variations and/or observable amounts of impurities in SmB6 crystals grown using both procedures affect the physical properties. From X-ray diffraction, neutron diffraction, and X-ray computed tomography experiments we observe that natural isotope containing (SmB6) and doubly isotope enriched ((154)Sm(11)B6) crystals prepared using aluminum flux contain co-crystallized, epitaxial aluminum. Further, a large, nearly stoichiometric crystal of SmB6 was successfully grown using the float-zone technique; upon continuing the zone melting, samarium vacancies were introduced. These samarium vacancies drastically alter the resistance and plateauing magnitude of the low temperature resistance compared to stoichiometric SmB6. These results highlight that impurities and compositional variations, even at low concentrations, must be considered when collecting/analyzing physical property data of SmB6. Finally, a more accurate samarium-154 coherent neutron scattering length, 8.9(1) fm, is reported.

Crystal growth, structure, and physical properties of Ln(Cu,Al)12 (Ln = Y, Ce, Pr, Sm, and Yb) and Ln(Cu, Ga)12 (Ln = Y, Gd-Er, and Yb).

Single crystals of Ln(Cu,Al)12 and Ln(Cu,Ga)12 compounds (Ln = Y, Ce-Nd, Sm, Gd-Ho, and Yb for Al and Ln = Y, Gd-Er, Yb for Ga) have been grown by flux-growth methods and characterized by means of single-crystal x-ray diffraction, complemented with microprobe analysis, magnetic susceptibility, resistivity and heat capacity measurements. Ln(Cu,Ga)12 and Ln(Cu,Al)12 of the ThMn12 structure type crystallize in the tetragonal I4/mmm space group with lattice parameters a approximately 8.59 Šand c approximately 5.15 Šand a approximately 8.75 Šand c approximately 5.13 Šfor Ga and Al containing compounds, respectively. For aluminium containing compounds, magnetic susceptibility data show Curie-Weiss paramagnetism in the Ce and Pr analogues down to 50 K with no magnetic ordering down to 3 K, whereas the Yb analogue shows a temperature-independent Pauli paramagnetism. Sm(Cu,Al)12 orders antiferromagnetically at T(N)approximately 5 K and interestingly exhibits Curie-Weiss behaviour down to 10 K with no Van Vleck contribution to the susceptibility. Specific heat data show that Ce(Cu,Al)12 is a heavy fermion antiferromagnet with T(N) approximately 2 K and with an electronic specific heat coefficient γ0 as large as 390 mJ K2 mol(-1). In addition, this is the first report of Pr(Cu,Al)12 and Sm(Cu,Al)12 showing an enhanced mass (approximately 80 and 120 mJ K(2) mol(-1)). For Ga containing analogues, magnetic susceptibility data also show the expected Curie-Weiss behaviour from Gd to Er, with the Yb analogue being once again a Pauli paramagnet. The antiferromagnetic transition temperatures range over 12.5, 13.5, 6.7, and 3.4 K for Gd, Tb, Dy, and Er. Metallic behaviour is observed down to 3 K for all Ga and Al analogues. A large positive magnetoresistance up to 150% at 9 T is also observed for Dy(Cu,Ga)12. The structure, magnetic, and transport properties of these compounds will be discussed.

Crystal growth, structure, and physical properties of Ln(Ag, Al, Si)2 (Ln = Ce and Gd).

Single crystals of CeM2 and GdM2 (M = Ag, Al, and Si) were grown by the flux growth technique and characterized by means of single crystal x-ray diffraction, magnetic susceptibility, resistivity, and heat capacity measurements. CeM2 and GdM2 crystallize in the tetragonal I4(1)/amd space group with the α-ThSi2 structure type with lattice parameters a ~4.2 Å and c ~14.4 Å. Curie-Weiss behavior is observed for both analogues with CeM2 ordering first ferromagnetically at 11 K with a second antiferromagnetic transition at 8.8 K while GdM2 orders antiferromagnetically at 24 K. Heat capacity measurements on CeM2 show two magnetic transitions at 10.8 and 8.8 K with an electronic specific heat coefficient, γ(0), of ~53 mJ K(-2) mol(-1). The entropy at the magnetic transition is less than the expected Rln2 for CeM2, reinforcing the assertions of an enhanced mass state and Kondo behavior being observed in the resistivity.

Crystal growth, structure, and physical properties of SmCu4Ga8.

Single crystals of SmCu4Ga8 have been grown using Ga flux and characterized by single-crystal X-ray diffraction. SmCu4Ga8, isostructural to SmZn11, crystallizes in the hexagonal P6/mmm (No. 191) space group, with Z = 3 and lattice parameters a = 8.865(2) A and c = 8.607(2) A. Magnetic susceptibility data show antiferromagnetic ordering at 3.3 K. Metallic behavior is observed in the temperature range 2-300 K. A large positive magnetoresistance (MR % = (rho H - rho 0)/rho 0 x 100) up to 40% is also observed near T N. In this paper, we present the structure and physical properties of SmCu4Ga8.

Discovery of the Griffiths phase in the itinerant magnetic semiconductor Fe1-xCoxS2.

Critical points that can be suppressed to zero temperature are interesting because quantum fluctuations have been shown to dramatically alter electron gas properties. Here, the metal formed by Co doping the paramagnetic insulator FeS2, Fe1-xCoxS2 is demonstrated to order ferromagnetically at x > xc = 0.01+/-0.005, where we observe unusual transport, magnetic, and thermodynamic properties. We show that this magnetic semiconductor undergoes a percolative magnetic transition with distinct similarities to the Griffiths phase, including singular behavior at xc and zero temperature.

NaV2O4: a quasi-1D metallic antiferromagnet with half-metallic chains.

NaV2O4 crystals were grown under high pressure using a NaCl flux, and the crystals were characterized with x-ray diffraction, electrical resistivity, heat capacity, and magnetization. The structure of NaV2O4 consists of double chains of edge-sharing VO6 octahedra. The resistivity is highly anisotropic, with the resistivity perpendicular to the chains more than 20 times greater than that parallel to the chains. Magnetically, the intrachain interactions are ferromagnetic and the interchain interactions are antiferromagnetic; 3D antiferromagnetic order is established at 140 K. First-principles electronic structure calculations indicate that the chains are half-metallic. Interestingly, the case of NaV2O4 seems to be a quasi-1D analogue of what was found for half-metallic materials.

Low-temperature susceptibility of the noncentrosymmetric superconductor CePt3Si.

We report ac susceptibility measurements of polycrystalline CePt(3)Si down to 60 mK and in applied fields up to 9 T. In a zero applied field, a full Meissner state emerges at temperatures T/T(c) < 0.3, where T(c) = 0.65 K is the onset transition temperature. Though transport measurements show a relatively high upper critical field B(c2) approximately 4-5 T, the low-temperature susceptibility chi(') is quite fragile to the applied field, with chi(') diminishing rapidly in fields of a few kG. Interestingly, the field dependence of chi(') is well described by the power law 4pichi(') + 1 = (B/B(c))(1/2), where B(c) is the field at which the onset of resistance is observed in transport measurements.

Synthesis, structure, and magnetoresistance of SmPd2Ga2.

Single crystals of a new ternary compound, SmPd(2)Ga(2), have been synthesized by flux growth methods. This compound adopts a tetragonal space group I4/mmm, Z = 2, with lattice parameters a = 4.2170(3) A and c = 10.4140(3) A. The crystal structure is composed of layers of isolated Sm atoms and layers of PdGa(4) edge-sharing tetrahedra alternating along the c-axis. The sample is metallic (d rho/dT > 0) with a weak temperature dependence above 100 K. This new material has physical properties similar to those of other Sm intermetallics and has, most notably, a large positive magnetoresistance at low temperatures. Magnetic measurements indicate that SmPd(2)Ga(2) is ferromagnetic with T(c) approximately 5 K.

Distribution and sources of nitrate-nitrogen in Kansas groundwater.

Kansas is primarily an agricultural state. Irrigation water and fertilizer use data show long- term increasing trends. Similarly, nitrate-N concentrations in groundwater show long-term increases and exceed the drinking-water standard of 10 mg/l in many areas. A statistical analysis of nitrate-N data collected for local and regional studies in Kansas from 1990 to 1998 (747 samples) found significant relationships between nitrate-N concentration with depth, age, and geographic location of wells. Sources of nitrate-N have been identified for 297 water samples by using nitrogen stable isotopes. Of these samples, 48% showed fertilizer sources (+2 to +8) and 34% showed either animal waste sources (+10 to +15 with nitrate-N greater than 10 mg/l) or indication that enrichment processes had occurred (+10 or above with variable nitrate-N) or both. Ultimate sources for nitrate include nonpoint sources associated with past farming and fertilization practices, and point sources such as animal feed lots, septic systems, and commercial fertilizer storage units. Detection of nitrate from various sources in aquifers of different depths in geographically varied areas of the state indicates that nonpoint and point sources currently impact and will continue to impact groundwater under current land uses.

High-temperature weak ferromagnetism in a low-density free-electron gas.

The magnetic properties of the ground state of a low-density free-electron gas in three dimensions have been the subject of theoretical speculation and controversy for seven decades. Not only is this a difficult theoretical problem to solve, it is also a problem which has not hitherto been directly addressed experimentally. Here we report measurements on electron-doped calcium hexaboride (CaB6) which, we argue, show that-at a density of 7× 1019 electrons cm-3-the ground state is ferromagnetically polarized with a saturation moment of 0.07 µB per electron. Surprisingly, the magnetic ordering temperature of this itinerant ferromagnet is 600 K, of the order of the Fermi temperature of the electron gas.