0000000000309266
AUTHOR
Jürgen Winterlik
Magnetic Heusler Compounds
Abstract Heusler compounds are a remarkable class of intermetallic materials with 1:1:1 (often called Half-Heusler) or 2:1:1 composition comprising more than 1500 members. New properties and potential fields of applications emerge constantly; the prediction of topological insulators is the most recent example. Surprisingly, the properties of many Heusler compounds can easily be predicted by the valence electron count or within a rigid band approach. The wide range of the multifunctional properties of Heusler compounds is reflected in extraordinary magnetooptical, magnetoelectronic, and magnetocaloric properties. Co 2 -Heusler compounds are predicted and proven half-metallic ferromagnets sho…
Disentangling the Mn moments on different sublattices in the half-metallic ferrimagnet Mn3−xCoxGa
Ferrimagnetic Mn3−xCoxGa compounds have been investigated by magnetic circular dichroism in x-ray absorption (XMCD). Compounds with x>0.5 crystallize in the CuHg2Ti structure. A tetragonal distortion of the cubic structure occurs for x≤0.5. For the cubic phase, magnetometry reveals a linearly increasing magnetization of 2x Bohr magnetons per formula unit obeying the generalized Slater–Pauling rule. XMCD confirms the ferrimagnetic character with Mn atoms occupying two different sublattices with antiparallel spin orientation and different degrees of spin localization and identifies the region 0.6<x≤0.8 as most promising for a high spin polarization at the Fermi level. Individual Mn moments on…
Challenge of magnetism in strongly correlated open-shell 2p systems.
We report on theoretical investigations of the exotic magnetism in rubidium sesquioxide ${\mathrm{Rb}}_{4}{\mathrm{O}}_{6}$, a model correlated system with an open $2p$ shell. Experimental investigations indicated that ${\mathrm{Rb}}_{4}{\mathrm{O}}_{6}$ is a magnetically frustrated insulator. The frustration is explained here by electronic structure calculations that incorporate the correlation between the oxygen $2p$ electrons and deal with the mixed-valent oxygen. This leads to a physical picture where the symmetry is reduced because one third of the oxygen in ${\mathrm{Rb}}_{4}{\mathrm{O}}_{6}$ is nonmagnetic while the remaining two thirds assemble in antiferromagnetic arrangements. A d…
Ni-based superconductor: Heusler compoundZrNi2Ga
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 He…
Structure-property relations in the distorted ordered double perovskite Sr2InReO6
The rock-salt ordered type double perovskite Sr${}_{2}$InReO${}_{6}$ is systematically investigated by means of powder x-ray diffraction, neutron powder diffraction, temperature-dependent electrical transport, heat capacity and magnetic susceptibility measurements, and electronic band structure calculations. The crystal structure of Sr${}_{2}$InReO${}_{6}$ is revised to be monoclinic (cryolite structure type, space group $P$2${}_{1}$/$n$) with all structural distortions according to the high-symmetry aristotype due to tilting of the InO${}_{6}$ and ReO${}_{6}$ octahedra, respectively. Sr${}_{2}$InReO${}_{6}$ is a Mott insulator with variable-range hopping. Two 5$d$ electrons are unpaired an…
Crystal Structure of New Heusler Compounds
Heusler compounds are promising materials in many fields of contemporary research. The spectrum of their possible applications ranges from magnetic and magneto-mechanical materials over semiconductors and thermoelectrics to superconductors. An important feature of the Heusler compounds is the possibility of controlling the valence electron concentration by partial substitution of elements. On the other hand, the properties also depend on the degree of ordering of the the crystal structure. In general, Heusler compounds crystallize in the Cu2MnAl-type structure but in many cases certain types of disorder are observed. In this paper a detailed description of the different types of disordered …
Structural, electronic, and magnetic properties of tetragonalMn3−xGa: Experiments and first-principles calculations
This work reports on the electronic, magnetic, and structural properties of the binary intermetallic compounds ${\mathrm{Mn}}_{3\ensuremath{-}x}\mathrm{Ga}$. The tetragonal ${\mathrm{DO}}_{22}$ phase of the ${\mathrm{Mn}}_{3\ensuremath{-}x}\mathrm{Ga}$ series, with $x$ varying from 0 to 1.0 in steps of $x=0.1$, was successfully synthesized and investigated. It was found that all these materials are hard magnetic, with energy products ranging from $10.1\phantom{\rule{0.3em}{0ex}}\mathrm{kJ}\phantom{\rule{0.2em}{0ex}}{\mathrm{m}}^{\ensuremath{-}3}$ for low Mn content $(x\ensuremath{\rightarrow}1)$ to $61.6\phantom{\rule{0.3em}{0ex}}\mathrm{kJ}\phantom{\rule{0.2em}{0ex}}{\mathrm{m}}^{\ensurema…
Ultrafine MnWO4 nanoparticles and their magnetic properties
Abstract Ultrafine nanoparticles of MnWO4, a compound showing low-temperature multiferroicity in the bulk, were synthesized by the polyol method. Studies using powder X-ray diffraction, scanning and transmission electron microscopy, dynamic light scattering, differential sedimentation and sorption techniques show the formation of a single-phase material, which is composed of MnWO4 nanoparticles with a prolate ellipsoidal shape (short axis of 4–5 nm, long axis of 11–12 nm) and an unprecedented high specific surface area of 166 m2 g−1. The as-prepared MnWO4 nanoparticles are readily crystalline after the liquid-phase synthesis. Temperature and field dependent magnetization measurements indica…
Superconductivity in palladium-based Heusler compounds
This work reports on four more Heusler superconductors: ${\text{Pd}}_{2}\text{ZrAl}$, ${\text{Pd}}_{2}\text{HfAl}$, ${\text{Pd}}_{2}\text{ZrIn}$, and ${\text{Pd}}_{2}\text{HfIn}$. These compounds exhibit superconducting transition temperatures ranging from 2.4--3.8 K as determined by resistivity measurements. According to their behavior in an external magnetic field, all compounds are type II bulk superconductors. The occurrence of superconductivity was predicted for these compounds using electronic structure calculations. The electronic structures exhibit van Hove singularities (saddle points) at the $L$ point. These lead to a maximum in the corresponding density of states and superconduct…
Electronic, structural, and magnetic properties of the half-metallic ferromagnetic quaternary Heusler compounds CoFeMnZ(Z=Al, Ga, Si, Ge)
The quaternary intermetallic Heusler compounds CoFeMn$Z$ ($Z=\text{Al}$, Ga, Si, or Ge) with $1:1:1:1$ stoichiometry were predicted to exhibit half-metallic ferromagnetism by ab initio electronic structure calculations. The compounds were synthesized using an arc-melting technique and the crystal structures were analyzed using x-ray powder diffraction. The electronic properties were investigated using hard x-ray photoelectron spectroscopy. The low-temperature magnetic moments, as determined from magnetization measurements, follow the Slater-Pauling rule, confirming the proposed high spin polarizations. All compounds have high Curie temperatures, allowing for applications at room temperature…
Tetragonal Heusler Compounds for Spintronics
With respect to the requirements of spin torque transfer (STT) materials, one the most promising materials families are the tunable tetragonal Heusler compounds based on Mn2YZ (Y=Co,Fe,Ni,Rh,...; Z=Al, Ga, Sn). They form the inverse cubic Heusler structure with three distinct magnetic sublattices, which allows a fine tuning of the magnetic properties. Starting with the stoichiometric Mn3Ga compound, we explored the complete phase diagram of Mn3-xYxZ (Y=Co, Fe, Ni and Z=Ga ). All series exhibit thermally stable magnetic properties. As we demonstrate, Mn3-xFexGa series, which are tetragonal over the whole range of compositions, are good as hard magnets, whereas magnetically more weak Mn3-xNix…
Iron-based Heusler compounds Fe2YZ: Comparison with theoretical predictions of the crystal structure and magnetic properties
The present work reports on the new soft ferromagnetic Heusler phases Fe${}_{2}$NiGe, Fe${}_{2}$CuGa, and Fe${}_{2}$CuAl, which in previous theoretical studies have been predicted to exist in a tetragonal Heusler structure. Together with the known phases Fe${}_{2}$CoGe and Fe${}_{2}$NiGa these materials have been synthesized and characterized by powder x-ray diffraction, ${}^{57}$Fe M\"ossbauer spectroscopy, superconducting quantum interference device, and energy-dispersive x-ray measurements. In particular M\"ossbauer spectroscopy was used to monitor the degree of local atomic order/disorder and to estimate magnetic moments at the Fe sites from the hyperfine fields. It is shown that in con…
Challenging the Prediction of Anionogenic Ferromagnetism for Rb4O6
It has been suggested that Rb4O6 should be a half-metallic ferromagnet with the magnetic moment carried by the hyperoxide anions and a Curie temperature above room temperature. In the present work,...
Are AuPdTM (T = Sc, Y and M = Al, Ga, In), Heusler Compounds Superconductors without Inversion Symmetry?
Heusler compounds with 2:1:1 stoichiometry either have a centrosymmetric Cu 2 MnAl structure or an Li 2 AgSb structure without a centre of inversion. The centrosymmetry is always lost in quaternary Heusler compounds with 1:1:1:1 stoichiometry and LiMgPdSn structure. This presents the possibility of realizing non-centrosymmetric superconductors in the family of Heusler compounds. The objective of this study is to search for and investigate such quaternary derivatives of Heusler compounds, particularly with respect to superconductivity. Several compounds were identified by carrying out calculations from first principles and superconductivity was observed in experiments conducted on AuPdScAl a…
Design Scheme of New Tetragonal Heusler Compounds for Spin-Transfer Torque Applications and its Experimental Realization
Band Jahn-Teller type structural instabilities of cubic Mn(2)YZ Heusler compounds causing tetragonal distortions can be predicted by ab initio band-structure calculations. This allows for identification of new Heusler materials with tunable magnetic and structural properties that can satisfy the demands for spintronic applications, such as in spin-transfer torque-based devices.
Element-specific magnetic moments and spin-resolved density of states in CoFeMnZ(Z=Al, Ga; Si, Ge)
Using circular dichroism in x-ray-absorption spectroscopy (XAS/XMCD), we determined element-specific magnetic moments and spin-resolved unoccupied densities of states (DOS) for Co, Fe, and Mn in the quaternary Heusler compounds CoFeMn$Z$ ($Z=\text{Al}$, Ga; Si, Ge). These compounds belong to a class of highly spin-polarized materials with cubic LiMgPdSn-type structure. Different structure models for the sublattice occupation leading to similar average magnetization values can be distinguished by comparison of element-specific moments with theory. We find that the compounds form similar structures, where Co, Fe, Mn, and $Z$ occupy the $X$, ${X}^{\ensuremath{'}}$, $Y$, and $Z$ sublattice of t…
Large Zero-Field Cooled Exchange-Bias in BulkMn2PtGa
We report a large exchange-bias (EB) effect after zero-field cooling the new tetragonal Heusler compound Mn2PtGa from the paramagnetic state. The first-principle calculation and the magnetic measurements reveal that Mn2PtGa orders ferrimagnetically with some ferromagnetic (FM) inclusions. We show that ferrimagnetic (FI) ordering is essential to isothermally induce the exchange anisotropy needed for the zero-field cooled (ZFC) EB during the virgin magnetization process. The complex magnetic behavior at low temperatures is characterized by the coexistence of a field induced irreversible magnetic behavior and a spin-glass-like phase. The field induced irreversibility originates from an unusual…
Superconductivity in the Heusler Family of Intermetallics
Several physical properties of the superconducting Heusler compounds, focusing on two systems (Y, Lu, Sc)Pd2Sn and APd2M, where A=Hf, Zr and M=Al, In, are summarized and compared. The analysis of the data shows the importance of the electron-phonon coupling for superconductivity in this family. We report the superconducting parameters of YPd2Sn, which has the highest Tc among all known Heusler superconductors.
Electronic, magnetic, and structural properties of the ferrimagnet Mn2CoSn
The magnetic ground state of the Heusler compound Mn${}_{2}$CoSn was predicted to be nearly half-metallic ferrimagnetic with a high spin polarization by ab initio electronic structure calculations. Mn${}_{2}$CoSn was synthesized, and the magnetic behavior of the compound was studied using a superconducting quantum interference device and x-ray magnetic circular dichroism. The experimental values were found to be in fair accordance with the theoretical predictions. The electronic structure and the crystal structure of Mn${}_{2}$CoSn were characterized comprehensively using x-ray powder diffraction, $^{119}\mathrm{Sn}$ M\"ossbauer spectroscopy, nuclear magnetic resonance, and hard x-ray photo…