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1.
J Phys Condens Matter ; 29(47): 475602, 2017 Nov 29.
Article in English | MEDLINE | ID: mdl-28972502

ABSTRACT

The electronic properties of the heavy metal superconductor [Formula: see text] are reported. The estimated superconducting parameters obtained from physical properties measurements indicate that [Formula: see text] is a BCS-type superconductor. Electronic band structure calculations show that Ir d-states dominate the Fermi level. A comparison of electronic band structures of [Formula: see text] and [Formula: see text] shows that the Ir-compound has a strong spin-orbit-coupling effect, which creates a complex Fermi surface.

2.
Proc Natl Acad Sci U S A ; 113(25): E3475-81, 2016 06 21.
Article in English | MEDLINE | ID: mdl-27274081

ABSTRACT

The recent discovery of extreme magnetoresistance (XMR) in LaSb introduced lanthanum monopnictides as a new platform to study this effect in the absence of broken inversion symmetry or protected linear band crossing. In this work, we report XMR in LaBi. Through a comparative study of magnetotransport effects in LaBi and LaSb, we construct a temperature-field phase diagram with triangular shape that illustrates how a magnetic field tunes the electronic behavior in these materials. We show that the triangular phase diagram can be generalized to other topological semimetals with different crystal structures and different chemical compositions. By comparing our experimental results to band structure calculations, we suggest that XMR in LaBi and LaSb originates from a combination of compensated electron-hole pockets and a particular orbital texture on the electron pocket. Such orbital texture is likely to be a generic feature of various topological semimetals, giving rise to their small residual resistivity at zero field and subject to strong scattering induced by a magnetic field.

3.
J Phys Condens Matter ; 27(18): 185701, 2015 May 13.
Article in English | MEDLINE | ID: mdl-25880601

ABSTRACT

We report the electronic properties of the cubic laves phase superconductor CaIr2(Tc = 5.8 K), in which the Ir atoms have a pyrochlore lattice. The estimated superconducting parameters obtained from magnetization and specific heat measurements indicate that CaIr2 is a weakly coupled BCS superconductor. Electronic band structure calculations show that the Ir d-states are dominant at the Fermi level, creating a complex Fermi surface that is impacted substantially by spin-orbit coupling.

5.
Nat Commun ; 6: 6489, 2015 Mar 06.
Article in English | MEDLINE | ID: mdl-25744553

ABSTRACT

The Zintl concept is important in solid-state chemistry to explain how some compounds that combine electropositive and main group elements can be stable at formulas that at their simplest level do not make any sense. The electronegative elements in such compounds form a polyatomic electron-accepting molecule inside the solid, a 'polyanion', that fills its available energy states with electrons from the electropositive elements to obey fundamental electron-counting rules. Here we use this concept to discover a large family of filled skutterudites based on the group 9 transition metals Co, Rh, and Ir, the alkali, alkaline-earth, and rare-earth elements, and Sb4 polyanions. Forty-three new filled skutterudites are reported, with 63 compositional variations--results that can be extended to the synthesis of hundreds of additional new compounds. Many interesting electronic and magnetic properties can be expected in future studies of these new compounds.

6.
J Am Chem Soc ; 137(2): 691-8, 2015 Jan 21.
Article in English | MEDLINE | ID: mdl-25539454

ABSTRACT

The discovery of n-type ferromagnetic semiconductors (n-FMSs) exhibiting high electrical conductivity and Curie temperature (Tc) above 300 K would dramatically improve semiconductor spintronics and pave the way for the fabrication of spin-based semiconducting devices. However, the realization of high-Tc n-FMSs and p-FMSs in conventional high-symmetry semiconductors has proven extremely difficult due to the strongly coupled and interacting magnetic and semiconducting sublattices. Here we show that decoupling the two functional sublattices in the low-symmetry semiconductor FeBi2Se4 enables unprecedented coexistence of high n-type electrical conduction and ferromagnetism with Tc ≈ 450 K. The structure of FeBi2Se4 consists of well-ordered magnetic sublattices built of [FenSe4n+2]∞ single-chain edge-sharing octahedra, coherently embedded within the three-dimensional Bi-rich semiconducting framework. Magnetotransport data reveal a negative magnetoresistance, indicating spin-polarization of itinerant conducting electrons. These findings demonstrate that decoupling magnetic and semiconducting sublattices allows access to high-Tc n- and p-FMSs as well as helps unveil the mechanism of carrier-mediated ferromagnetism in spintronic materials.

7.
Nature ; 514(7521): 205-8, 2014 Oct 09.
Article in English | MEDLINE | ID: mdl-25219849

ABSTRACT

Magnetoresistance is the change in a material's electrical resistance in response to an applied magnetic field. Materials with large magnetoresistance have found use as magnetic sensors, in magnetic memory, and in hard drives at room temperature, and their rarity has motivated many fundamental studies in materials physics at low temperatures. Here we report the observation of an extremely large positive magnetoresistance at low temperatures in the non-magnetic layered transition-metal dichalcogenide WTe2: 452,700 per cent at 4.5 kelvins in a magnetic field of 14.7 teslas, and 13 million per cent at 0.53 kelvins in a magnetic field of 60 teslas. In contrast with other materials, there is no saturation of the magnetoresistance value even at very high applied fields. Determination of the origin and consequences of this effect, and the fabrication of thin films, nanostructures and devices based on the extremely large positive magnetoresistance of WTe2, will represent a significant new direction in the study of magnetoresistivity.

8.
Chem Commun (Camb) ; 50(2): 201-3, 2014 Jan 07.
Article in English | MEDLINE | ID: mdl-24217186

ABSTRACT

Polypropylene grafted maleic anhydride (PP-MA, 2500 g mole(-1)) has demonstrated its unique capability to synthesize 1-D ferromagnetic hard (292.7 Oe) γ-Fe2O3 nanochains made of ~24 nm nanoparticles vs. PP-MA with 8000 g mole(-1) for the synthesis of 1-D ferromagnetic soft (70.5 Oe) γ-Fe2O3 nanochains (30 nm) made of flowerlike nanoparticles.

9.
Phys Chem Chem Phys ; 15(26): 10866-75, 2013 Jul 14.
Article in English | MEDLINE | ID: mdl-23698645

ABSTRACT

Phosphoric acid doped conductive polyaniline (PANI) polymer nanocomposites (PNCs) reinforced with silicon nanopowders have been successfully synthesized using a facile surface initiated polymerization (SIP) method. The chemical structures of the nanocomposites are characterized using Fourier transform infrared (FT-IR) spectroscopy. The enhanced thermal stability of the silicon-PANI PNCs compared with pure PANI is obtained using thermogravimetric analysis (TGA). The obtained optical band gap of the PNCs using Ultraviolet-visible diffuse reflectance spectroscopy (UV-vis DRS) decreases with increasing silicon loading. The dielectric properties of the PNCs are strongly related to the silicon loading level. Temperature dependent resistivity analysis reveals a quasi 3-D variable range hopping (VRH) electrical conduction mechanism for the synthesized PNCs. Room temperature giant magnetoresistance (GMR) is observed in the synthesized non-magnetic nanocomposites and analyzed using the wave-function shrinkage model.

10.
Inorg Chem ; 52(9): 5055-62, 2013 May 06.
Article in English | MEDLINE | ID: mdl-23600622

ABSTRACT

Crystal growth, structure determination, and magnetic properties of LnCr2Al(20-x)Fe(x) (Ln = La, Gd, Yb) adopting the CeCr2Al20 structure type with space group Fd3m, a ∼ 14.5 Å, are reported. Single crystal X-ray diffraction and Mössbauer spectroscopy are employed to fully characterize the crystal structure of LnCr2Al(20-x)Fe(x) (Ln = La, Gd, Yb). LnCr2Al(20-x)Fe(x) (Ln = La, Gd, Yb) are the first pseudoternaries adopting the CeCr2Al20 structure type with a transition metal occupying the main group site. The Yb analogues are Pauli paramagnets with the Yb ion adopting an electronic configuration close to Yb(2+), while the Gd analogues show paramagnetic behavior with no magnetic order down to 3 K.

11.
Nanoscale ; 5(5): 1825-30, 2013 Mar 07.
Article in English | MEDLINE | ID: mdl-23377290

ABSTRACT

Contrary to the helical carbon structure from pure cotton fabrics under microwave heating and radical oxidized ignition of nanoparticles from conventional heating, magnetic carbon tubular nanocomposite fabrics decorated with uniformly dispersed Co-Co(3)O(4) nanoparticles were successfully synthesized via a microwave heating process using cotton fabric and inorganic salt as precursors, which have shown better anti-corrosive performance and demonstrated great potential as novel electrochemical pseudocapacitor electrode.

12.
Inorg Chem ; 52(6): 3198-206, 2013 Mar 18.
Article in English | MEDLINE | ID: mdl-23437910

ABSTRACT

Ln2Ru3Al15 (Ln = Ce, Gd) have been synthesized, and the competition between the growth of Ce2Ru3Al15 and CeRu2Al10 has been studied. The structure of Ce2Ru3Al15 was modified from the previously reported Ce2Ru3Al15 structure, and the structure of Gd2Ru3Al15 was determined for the first time. The magnetic and transport properties of Ln2Ru3Al15 were measured and compared to the properties of LnRu2Al10. Gd2Ru3Al15 orders antiferromagnetically at 21.0 K with a spin reorientation at 4.1 K and has a positive paramagnetic Curie-Weiss temperature of 11.5(17) K, suggesting strong ferromagnetic interactions within the structure. Ce2Ru3Al15 displays two low-temperature magnetic transitions at 3.7 and 3.1 K, the first of which is believed to be an antiferromagnetic ordering, with a θN of -7(3) K and a reduced moment of 2.33(4) µB/mol-Ce. Furthermore, the low-temperature magnetic and transport properties display the effects of Kondo screening of the magnetic moments. While structurally related, the properties of Ce2Ru3Al15 do not display the same anomalous features observed in CeRu2Al10.

13.
Chem Commun (Camb) ; 49(26): 2679-81, 2013 Apr 04.
Article in English | MEDLINE | ID: mdl-23435465

ABSTRACT

A novel function of maleic anhydride grafted polypropylene (PP) with different backbone chain-lengths was demonstrated, i.e., in controlling the cobalt morphologies (dispersed polyhedral vs. assembled chain nanostructure), crystalline structures (ε- vs. ß-phase), and magnetic property (242 vs. 808 Oe) in the synthesized magnetic PP nanocomposites.


Subject(s)
Cobalt/chemistry , Maleic Anhydrides/chemistry , Metal Nanoparticles/chemistry , Nanocomposites/chemistry , Polypropylenes/chemistry , Magnetic Fields , Particle Size , Surface Properties
14.
J Am Chem Soc ; 135(7): 2748-58, 2013 Feb 20.
Article in English | MEDLINE | ID: mdl-23350732

ABSTRACT

We present the structure of Ln(30)Ru(4+x)Sn(31-y) (Ln = Gd, Dy) and the anisotropic resistivity, magnetization, thermopower, and thermal conductivity of single crystal Ln(30)Ru(4+x)Sn(31-y) (Ln = Gd, Tb). Gd(30)Ru(4.92)Sn(30.54) crystallizes in a new structure-type with space group Pnnm and dimensions of a = 11.784(1) Å, b = 24.717(1) Å, and c = 11.651(2) Å, and V = 3394(1) Å(3). Magnetic anisotropy and highly anisotropic electrical transport behavior were observed in the single crystals of Gd(30)Ru(4.92)Sn(30.54) and Tb(30)Ru(6)Sn(29.5). Additionally, the lattice thermal conductivity of Tb(30)Ru(6)Sn(29.5) is quite low, and a comparison is made to other Sn-containing compounds.

15.
Chem Commun (Camb) ; 49(3): 258-60, 2013 Jan 11.
Article in English | MEDLINE | ID: mdl-23172110

ABSTRACT

Magnetic carbon nanostructures from microwave assisted- and conventional-pyrolysis processes are compared. Unlike graphitized carbon shells from conventional heating, different carbon shell morphologies including nanotubes, nanoflakes and amorphous carbon were observed. Crystalline iron and cementite were observed in the magnetic core, different from a single cementite phase from the conventional process.


Subject(s)
Carbon/chemistry , Magnetics , Microwaves , Nanostructures/chemistry , Magnetite Nanoparticles/chemistry , Nanotubes/chemistry , Temperature
16.
Inorg Chem ; 51(19): 10193-202, 2012 Oct 01.
Article in English | MEDLINE | ID: mdl-22963342

ABSTRACT

Ln(Cu,Al,Ga)(13-x) (Ln = La-Pr, and Eu; x ~ 0.2) were synthesized by a combined Al/Ga flux. Single crystal X-ray and neutron diffraction experiments revealed that these compounds crystallize in the NaZn(13) structure-type (space group Fm3[overline]c) with lattice parameters of a ~ 12 Å, V ~ 1600 Å, and Z ~ 8. Our final neutron models led us to conclude that Cu is occupationally disordered on the 8b Wyckoff site while Cu, Al, and Ga are substitutionally disordered on the 96i Wyckoff site of this well-known structure-type. The magnetic susceptibility data show that Ce(Cu,Al,Ga)(13-x) and Pr(Cu,Al,Ga)(13-x) exhibit paramagnetic behavior down to the lowest temperatures measured while Eu(Cu,Al,Ga)(13-x) displays ferromagnetic behavior below 6 K. Eu(Cu,Al)(13-x) was prepared via arc-melting and orders ferromagnetically below 8 K. The magnetocaloric properties of Eu(Cu,Al,Ga)(13-x) and Eu(Cu,Al)(13-x) were measured and compared. Additionally, an enhanced value of the Sommerfeld coefficient (γ = 356 mJ/mol-K(2)) was determined for Pr(Cu,Al,Ga)(13-x). Herein, we present the synthesis, structural refinement details, and physical properties of Ln(Cu,Al,Ga)(13-x) (Ln = La-Pr, and Eu) and Eu(Cu,Al)(13-x).

17.
ACS Appl Mater Interfaces ; 4(10): 5613-24, 2012 Oct 24.
Article in English | MEDLINE | ID: mdl-22985210

ABSTRACT

Magnetic epoxy polymer nanocomposites (PNCs) reinforced with magnetite (Fe(3)O(4)) nanoparticles (NPs) have been prepared at different particle loading levels. The particle surface functionality tuned by conductive polyaniline (PANI) is achieved via a surface initiated polymerization (SIP) approach. The effects of nanoparticle loading, surface functionality, and temperature on both the viscosity and storage/loss modulus of liquid epoxy resin suspensions and the physicochemical properties of the cured solid PNCs are systematically investigated. The glass transition temperature (T(g)) of the cured epoxy filled with the functionalized NPs has shifted to the higher temperature in the dynamic mechanical analysis (DMA) compared with that of the cured pure epoxy. Enhanced mechanical properties of the cured epoxy PNCs filled with the functionalized NPs are observed in the tensile test compared with that of the cured pure epoxy and cured epoxy PNCs filled with as-received NPs. The uniform NP distribution in the cured epoxy PNCs filled with functionalized NPs is observed by scanning electron microscope (SEM). These magnetic epoxy PNCs show the good magnetic properties and can be attached by a permanent magnet. Enhanced interfacial interaction between NPs and epoxy is revealed in the fracture surface analysis. The PNCs formation mechanism is also interpreted from the comprehensive analysis based on the TGA, DSC, and FTIR in this work.

18.
J Am Chem Soc ; 134(31): 12998-3009, 2012 Aug 08.
Article in English | MEDLINE | ID: mdl-22849326

ABSTRACT

New distorted variants of the cubic BaHg11 structure type have been synthesized in Ga flux. Multiple phases of CePd3+xGa8-x, which include an orthorhombic Pmmn structure (x = 3.21(2)), a rhombohedral R3m structure (x = 3.13(4)), and a cubic Fm3m superstructure (x = 2.69(6)), form preferentially depending on reaction cooling rate and isolation temperature. Differential thermal analysis and in situ temperature-dependent powder X-ray diffraction patterns show a reversible phase transition at approximately 640 °C between the low temperature orthorhombic and rhombohedral structures and the high temperature cubic superstructure. Single crystal X-ray diffraction experiments indicate that the general structure of BaHg11, including the intersecting planes of a kagomé-type arrangement of Ce atoms, is only slightly distorted in the low temperature phases. A combination of Kondo, crystal electric field, and magnetic frustration effects may be present, resulting in low temperature anomalies in magnetic susceptibility, electrical resistivity, and heat capacity measurements. In addition to CePd3+xGa8-x, the rare earth analogues REPd3+xGa8-x, RE = La, Nd, Sm, Tm, and Yb, were successfully synthesized and also crystallize in one of the lower symmetry space groups.

20.
J Am Chem Soc ; 134(13): 5965-73, 2012 Apr 04.
Article in English | MEDLINE | ID: mdl-22375963

ABSTRACT

The discovery of novel materials with low thermal conductivity is paramount to improving the efficiency of thermoelectric devices. As lattice thermal conductivity is inversely linked to unit cell complexity, we set out to synthesize a highly complex crystalline material with glasslike thermal conductivity. Here we present the structure, transport properties, heat capacity, and magnetization of single-crystal Gd(117)Co(56)Sn(112), a complex material with a primitive unit cell volume of ~6858 Å(3) and ~285 atoms per primitive unit cell (1140 atoms per face-centered cubic unit cell). The room temperature lattice thermal conductivity of this material is κ(L) = 0.28 W/(m·K) and represents one of the lowest ever reported for a nonglassy or nonionically conducting bulk solid. Furthermore, this material exhibits low resistivity at room temperature, and thus represents a true physical system that approaches the ideal phonon glass-electron crystal.

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