Anomalous transport properties of the half-metallic ferromagnets Co 2 TiSi, Co 2 TiGe and Co 2 TiSn
In this work the theoretical and experimental investigations of Co2TiZ (Z = Si, Ge, or Sn) compounds are reported. Half-metallic ferromagnetism is predicted for all three compounds with only two bands crossing the Fermi energy in the majority channel. The magnetic moments fulfill the Slater-Pauling rule and the Curie temperatures are well above room temperature. All compounds show a metallic like resistivity for low temperatures up to their Curie temperature, above the resistivity changes to semiconducting like behavior. A large negative magnetoresistance of 55% is observed for Co2TiSn at room temperature in an applied magnetic field of 4T which is comparable to the large negative magnetore…
Shape-Dependence of Pd Nanocrystal Carburization during Acetylene Hydrogenation
This interdisciplinary work combines the use of shape- and size-defined Pd nanocrystals (cubes of 10 and 18 nm, and octahedra of 37 nm) with in situ techniques and DFT calculations to unravel the dynamic phenomena with respect to Pd reconstruction taking place during acetylene hydrogenation. Notably, it was found that the reacting Pd surface evolved at a different pace depending on the shape of the Pd nanocrystals, due to their specific propensity to form carbides under reaction conditions. Indeed, Pd cubes (Pd(100)) reacted with acetylene to form a PdC0.13 phase at a rate roughly 6-fold higher than that of octahedra (Pd(111)), resulting in nanocrystals with different degrees of carburizati…
Itinerant half-metallic ferromagnetsCo2TiZ(Z=Si, Ge, Sn):Ab initiocalculations and measurement of the electronic structure and transport properties
This work reports on ab initio calculations and experiments on the half-metallic ferromagnetic Heusler compounds ${\text{Co}}_{2}\text{Ti}Z$ $(Z=\text{Si},\text{ }\text{Ge},\text{ }\text{Sn})$. Aim is a comprehensive study of the electronic-structure and thermoelectric properties. The impact of the variation in the main group element $Z$ on those properties is discussed. X-ray diffraction was performed on the compounds and the lattice parameters are compared to other ${\text{Co}}_{2}$-based compounds. Hard x-ray photoemission measurements were carried out and the results are compared to the calculated electronic structure. The experimentally determined electronic structure, magnetic propert…
Zn-substituted iron oxide nanoparticles from thermal decomposition and their thermally treated derivatives for magnetic solid-phase extraction
Abstract Controlled thermal decomposition of zinc and iron acetylacetonates in the presence of oleic acid and oleylamine provided surfactant-capped magnetic nanoparticles with narrow size distribution and the mean diameter of ≈15 nm. The combined study by XRD, XRF and Mossbauer spectroscopy revealed three important features of the as-prepared nanoparticles. First, the actual ratio of Zn:Fe was considerably lower in the product compared to the initial ratio of metal precursors (0.14 vs. 0.50). Second, a pure stoichiometric Zn-doped magnetite system, specifically of the composition Zn0.37Fe2.63O4, with no signatures of oxidation to maghemite was formed. Third, Zn2+ ions were distributed at bo…
Half-Heusler superlattices as model systems for nanostructured thermoelectrics
The efficiency of thermoelectric materials is directly related to the dimensionless figure of merit , therefore, one of the means to improve ZT is to reduce the thermal conductivity. Our research focuses on half-Heusler superlattices (SLs) and the relationship between the SL period and the thermal conductivity. The cross-plane thermal conductivity of DC-sputtered TiNiSn/HfNiSn SLs was measured by the 3 method at room temperature and a clear reduction of was achieved for all SL periods, in particular for periods smaller than 20 nm. Moreover, the thermal conductivities of TiNiSn and HfNiSn single films display reduced values compared to the literature data for bulk materials. Furthermore, we …
Thermal conductivity of thermoelectric Al-substituted ZnO thin films
ZnO:Al thin films with a low electrical resistivity were grown by magnetron sputtering on sapphire substrates. The cross-plane thermal conductivity (κ = 4.5 ± 1.3 W/mK) at room temperature is almost one order of magnitude lower than for bulk materials. The thermoelectric figure of merit ZT at elevated temperatures was estimated from in-plane power factor and the cross-plane thermal conductivity at room temperature. It is expected that the thermal conductivity drops with increasing temperature and is lower in-plane than cross-plane. Consequently, the thin film ZT is at least three times higher than for bulk samples at intermediate temperatures. (© 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinh…
Half-Heusler materials as model systems for phase-separated thermoelectrics
Semiconducting half-Heusler compounds based on NiSn and CoSb have attracted attention because of their good performance as thermoelectric materials. Nanostructuring of the materials was experimentally established through phase separation in (T1−x′Tx″)T(M1−yMy′) alloys when mixing different transition metals (T, T′, T″) or main group elements (M, M′). The electric transport properties of such alloys depend not only on their micro- or nanostructure but also on the atomic-scale electronic structure. In the present work, the influence of the band structure and density of states on the electronic transport and thermoelectric properties is investigated in detail for the constituents of phase-sepa…
Tuning the carrier concentration for thermoelectrical application in the quaternary Heusler compound Co2TiAl(1−x)Six
The family of half-metallic ferromagnets Co2TiZ exhibits exceptional transport properties. The investigated compounds Co2TiAl(1−x)Six (x = 0.25, 0.5, 0.75) show Curie temperatures (TCs) that vary between 250 and 350 K, depending on the composition. Above TC the Seebeck coefficient remains constant. This makes them promising candidates for thermoelectric devices such as thermocouples with a tunable working range. The electrical resistivity data show an anomaly at TC which is attributed to changes in the electronic structure and therefore in the carrier concentration.
Thermal conductivity of half-Heusler superlattices
Thin films and superlattices (SLs) of TiNiSn and ZrHfNiSn layers have been grown by dc magnetron sputtering on MgO (100) substrates to reduce the thermal conductivity, aiming for improvement of the thermoelectric figure of merit ZT. The thermal conductivity of 1 Wm−1K−1 was measured by the differential 3ω method for an SL with a periodicity of 8.8 nm. In addition to x-ray diffraction analysis of the SL crystal structure, smooth interfaces were confirmed by scanning/transmission electron microscopy.
Seebeck coefficients of half-metallic ferromagnets
In this report the Co2 based Heusler compounds are discussed as potential materials for spin voltage generation. The compounds were synthesized by arcmelting and consequent annealing. Band structure calculations were performed and revealed the compounds to be half-metallic ferromagnets. Magnetometry was performed on the samples and the Curie temperatures and the magnetic moments were determined. The Seebeck coefficients were measured from low to ambient temperatures for all compounds. For selected compounds high temperature measurements up to 900 K were performed.
Investigation of the Thermoelectric Properties of the Series TiCo1-xNixSnxSb1-x
The effect of the simultaneous substitution of cobalt by nickel and antimony by tin in the solid solution TiCo1–xNixSnxSb1–x was systematically investigated. The number of valence electrons does not change by this substitution and therefore the resistivity stays semimetallic or semiconducting. The series were synthesized by arcmelting and the thermoelectric properties were determined. It was found out that the substitution of cobalt and antimony by nickel and tin reduces the thermal conductivity to 2 W·m–1·K–1 at 400 K. The reduction is caused by titanium rich prolate micro structures that were found by energy dispersive X-ray spectroscopy investigations. The Seebeck coefficient and the res…
Doped semiconductors as half-metallic materials: Experiments and first-principles calculations ofCoTi1−xMxSb(M=Sc, V, Cr, Mn, Fe)
This work reports experiments and first-principles calculations on the substitutional semiconducting $C{1}_{b}$ compound $\mathrm{Co}{\mathrm{Ti}}_{1\ensuremath{-}x}{M}_{x}\mathrm{Sb}$. Diluted magnetic semiconductors have been prepared by substituting titanium in the semiconducting compound CoTiSb by other $3d$ transition elements $M$. Self-consistent calculations of the electronic structure predict some of the materials to be half-metallic ferromagnets. The structural, electronic, electric, and magnetic properties of the pure and substituted materials have been investigated. It is found from the experiments that substitution of up to 10% Ti by Fe, Mn, Cr, and V does not affect the crystal…