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Exploration of the gold-rich part of the ternary Gd-Au-Al system afforded the intermetallic compound GdAu 6.75-x Al 0.5+x (x ≈ 0.54) which was structurally characterized by single crystal X-ray diffraction (Pnma, a = 18.7847(4) Å, b = 23.8208(5) Å, c = 5.3010(1) Å). GdAu 6.75-x Al 0.5+x crystallizes in a previously unknown structure type featuring layers of Gd 2 (Au, Al) 29 and Gd 2 (Au, Al) 28 clusters which are arranged as in a close-packing parallel to the ac plane. The Gd substructure corresponds to slightly corrugated 3 6 nets (d Gd-Gd  = 5.30-5.41 Å) which are stacked on top of each other along the b direction with alternating short (5.4, 5.6 Å, within layers) and long distances (6.4 Å, between layers). The title compound has been discussed with respect to a quasicrystal approximant (1/1 AC) GdAu 5.3 Al in the same system. The magnetic properties of GdAu 6.75-x Al 0.5+x were found to be reminiscent to those of some ternary ACs, with sharp peaks in the temperature dependent magnetization, and metamagnetic-like transitions. The material becomes antiferromagnetic below 25 K; magnetometry results suggest that the antiferromagnetic state is composed of ferromagnetic ac planes, coupled antiferromagnetically along the b direction., (© 2022. The Author(s).)

Dense systems of magnetic nanoparticles may exhibit dipolar collective behavior. However, two fundamental questions remain unsolved: i) whether the transition temperature may be affected by the particle anisotropy or it is essentially determined by the intensity of the interparticle dipolar interactions, and ii) what is the minimum ratio of dipole-dipole interaction (E dd ) to nanoparticle anisotropy (K ef V, anisotropy⋅volume) energies necessary to crossover from individual to collective behavior. A series of particle assemblies with similarly intense dipolar interactions but widely varying anisotropy is studied. The K ef  is tuned through different degrees of cobalt-doping in maghemite nanoparticles, resulting in a variation of nearly an order of magnitude. All the bare particle compacts display collective behavior, except the one made with the highest anisotropy particles, which presents "marginal" features. Thus, a threshold of K ef V/E dd  ≈ 130 to suppress collective behavior is derived, in good agreement with Monte Carlo simulations. This translates into a crossover value of ≈1.7 for the easily accessible parameter T MAX (interacting)/T MAX (non-interacting) (ratio of the peak temperatures of the zero-field-cooled magnetization curves of interacting and dilute particle systems), which is successfully tested against the literature to predict the individual-like/collective behavior of any given interacting particle assembly comprising relatively uniform particles., (© 2022 The Authors. Small published by Wiley-VCH GmbH.)

The non-equilibrium dynamics of the superspin glass state of a dense assembly of ~ 2 nm MnFe 2 O 4 nanoparticles was investigated by means of magnetization, ac susceptibility and Mössbauer spectroscopy measurements and compared to the results of Monte Carlo simulations for a mesoscopic model that includes particles morphology and interparticle interactions. The zero-field cooled (ZFC), thermoremanent (TRM), and isothermal remanent magnetization (IRM) were recorded after specific cooling protocols and compared to those of archetypal spin glasses and their dimensionality. The system is found to display glassy magnetic features. We illustrate in detail, by a number of experiments, the dynamical properties of the low-temperature superspin glass phase. We observe that these glassy features are quite similar to those of atomic spin glasses. Some differences are observed, and interestingly, the non-atomic nature of the superspin glass is also reflected by an observed superspin dimensionality crossover. Monte Carlo simulations-that explicitly take into account core and surface contributions to the magnetic properties of these ultrasmall nanoparticles in direct contact, as well as interparticle interactions-evidence effects of the interplay between (intraparticle) core/surface exchange coupling and (interparticle) dipolar and exchange interactions.

Random field induced spontaneous excess moments appear in field cooled single crystals of diluted Ising antiferromagnets. Here we report results from low temperature measurements of field cooled (including zero field) magnetic hysteresis loops parallel and perpendicular to the c-axis of a single crystal of composition Fe 0.6 Zn 0.4 F 2 . We find that weak static ferromagnetic excess moments attained on field cooling give rise to an apparent exchange bias of the magnetic hysteresis loops, whose magnitude is controlled by temperature and the strength and direction of the cooling field. Random field induced temporal excess moments only become observable in cooling fields larger than 1 T applied along the c-axis direction of the Fe 0.6 Zn 0.4 F 2 single crystal.

The anisotropic antiferromagnet FeF 2 has been extensively used as an antiferromagnetic layer to induce exchange bias effects in ferromagnetic/antiferromagnetic bilayers and heterostructures. In this work, an apparent exchange bias occurring in the low temperature hysteresis loops of FeF 2 single crystals is investigated. A detailed investigation of the hysteresis and remnant magnetization indicates that the observation of an apparent exchange bias in FeF 2 stems from an intrinsic excess moment associated with a distortion of the antiferromagnetic structure of piezomagnetic origin.

The properties of natural and artificial assemblies of interacting elements, ranging from Quarks to Galaxies, are at the heart of Physics. The collective response and dynamics of such assemblies are dictated by the intrinsic dynamical properties of the building blocks, the nature of their interactions and topological constraints. Here we report on the relaxation dynamics of the magnetization of artificial assemblies of mesoscopic spins. In our model nano-magnetic system - square artificial spin ice - we are able to control the geometrical arrangement and interaction strength between the magnetically interacting building blocks by means of nano-lithography. Using time resolved magnetometry we show that the relaxation process can be described using the Kohlrausch law and that the extracted temperature dependent relaxation times of the assemblies follow the Vogel-Fulcher law. The results provide insight into the relaxation dynamics of mesoscopic nano-magnetic model systems, with adjustable energy and time scales, and demonstrates that these can serve as an ideal playground for the studies of collective dynamics and relaxations.

Single crystals of the multiferroic double-perovskite Pb2MnWO6 have been synthesized and their structural, thermal, magnetic and dielectric properties studied in detail. Pure perovskite-phase formation and stoichiometric chemical composition of the as-grown crystals are confirmed by X-ray single-crystal and powder diffraction techniques as well as energy-dispersive X-ray and inductively coupled plasma mass spectrometry. Detailed structural analyses reveal that the crystals experience a structural phase transition from the cubic space group (s.g.) Fm3̅m to an orthorhombic structure in s.g. Pn21a at about 460 K. Dielectric data suggest that a ferrielectric phase transition takes place at that same temperature, in contrast to earlier results on polycrystalline samples, which reported a transition to s.g. Pnma and an antiferroelectric low-temperature phase. Magnetic susceptibility measurements indicate that a frustrated antiferromagnetic phase emerges below 8 K. Density functional theory based calculations confirm that the cationic order between Mn and W is favorable. The lowest total energy was found for an antiferromagnetically ordered state. However, analyses of the calculated exchange parameters revealed strongly competing antiferromagnetic interactions. The large distance between the magnetic atoms, together with magnetic frustration, is shown to be the main reason for the low value of the ordering temperature observed experimentally. We discuss the structure-property relationships in Pb2MnWO6 and compare these observations to reported results on related Pb2BWO6 perovskites with different B cations.

A novel synthesis method, "arc-melting-self-flux", has been developed and a series of five Tsai-type 1/1 approximant crystals in the Tb-Au-Si system have been synthesized. The synthesis method, by employing a temperature program which oscillates near the melting and nucleation points of the approximants, has provided high-quality and large single crystals in comparison to those obtained from the standard arc-melting-annealing and self-flux methods. The atomic structures of the approximants have been determined from single-crystal X-ray diffraction data and described using concentric atomic clusters with icosahedral symmetry. The compounds are nearly isostructural with subtle variations; two types of atomic clusters which mainly vary at their cluster centers are observed. One type contains a Tb site at the center, and the other contains a disordered tetrahedron decorated with Au/Si mixed sites. Both cluster types can be found coexisting in the approximants. The compounds have different average weighted ratios of central Tb to disordered tetrahedron in the bulk material. Furthermore, a strategy for chemically tuning magnetic behavior is presented. Magnetic property measurements on the approximants revealed that the magnetic transition temperature (Tc) decreases as the occupancy of the central Tb site increases. Tc decreased from 11.5 K for 0% occupancy of the central Tb to 8 K for 100% occupancy. Enhanced magneto crystalline anisotropy is observed for the approximants with higher central Tb occupancy in comparison to their low central Tb occupancy counterparts. Hence, the previously reported "ferrimagnetic-like" magnetic structure model remains valid.

A unidirectional anisotropy appears in field cooled samples of dilute magnetic alloys at temperatures well below the cusp temperature of the zero field cooled magnetization curve. Magnetization measurements on a Cu(13.5 at% Mn) sample show that this anisotropy is essentially temperature independent and acts on a temperature dependent excess magnetization, ΔM. The anisotropy can be partially or fully transferred from being locked to the direction of the cooling field at lower fields to becoming locked to the direction of ΔM at larger fields, thus instead appearing as a uniaxial anisotropy. This introduces a deceiving division of the anisotropy into a superposition of a unidirectional and a uniaxial part. This two faced nature of the anisotropy has been empirically scrutinized and concluded to originate from one and the same exchange mechanism: the Dzyaloshinsky-Moriya interaction.

The hydride NdGaH1+x (x ≈ 0.66) and its deuterized analogue were obtained by sintering the Zintl phase NdGa with the CrB structure in a hydrogen atmosphere at pressures of 10-20 bar and temperatures near 300 °C. The system NdGa/NdGaH1+x exhibits reversible H storage capability. H uptake and release were investigated by kinetic absorption measurements and thermal desorption mass spectroscopy, which showed a maximum H concentration corresponding to "NdGaH2" (0.93 wt % H) and a two-step desorption process, respectively. The crystal structure of NdGaH1+x was characterized by neutron diffraction (P21/m, a = 4.1103(7), b = 4.1662(7), c = 6.464(1) Å, β = 108.61(1)° Z = 2). H incorporates in NdGa by occupying two distinct positions, H1 and H2. H1 is coordinated in a tetrahedral fashion by Nd atoms. The H2 position displays flexible occupancy, and H2 atoms attain a trigonal bipyramidal coordination by centering a triangle of Nd atoms and bridging two Ga atoms. The phase stability and electronic structure of NdGaH1+x were analyzed by first-principles DFT calculations. NdGaH1H2 (NdGaH2) may be expressed as Nd(3+)(H1(-))[GaH2](2-). The two-dimensional polyanion [GaH](2-) features linear -H-Ga-H-Ga- chains with alternating short (1.8 Å) and long (2.4 Å) Ga-H distances, which resembles a Peierls distortion. H2 deficiency (x < 1) results in the fragmentation of chains. For x = 0.66 arrangements with five-atom moieties, Ga-H-Ga-H-Ga are energetically most favorable. From magnetic measurements, the Curie-Weiss constant and effective magnetic moment of NdGaH1.66 were obtained. The former indicates antiferromagnetic interactions, and the latter attains a value of ∼3.6 μB, which is typical for compounds containing Nd(3+) ions.

The question of the dominant interparticle magnetic interaction type in random closely packed assemblies of different diameter (6.2-11.5 nm) bare maghemite nanoparticles (NPs) is addressed. Single-particle magnetic properties such as particle anisotropy and exchange bias field are first of all studied in dilute (reference) systems of these same NPs, where interparticle interactions are neglible. Substantial surface spin disorder is revealed in all particles except the smallest, viz. for diameters d = 8-11.5 nm but not for d = 6.2-6.3 nm. X-ray diffraction analysis points to a crystallographic origin of this effect. The study of closely packed assemblies of the d ≥ 8 nm particles observes collective (superspin) freezing that clearly appears to be governed by interparticle dipole interactions. However, the dense assemblies of the smallest particles exhibit freezing temperatures that are higher than expected from a simple (dipole) extrapolation of the corresponding temperatures found in the d ≥ 8 nm assemblies. It is suggested that the nature of the dominant interparticle interaction in these smaller particle assemblies is superexchange, whereby the lack of significant surface spin disorder allows this mechanism to become important at the level of interacting superspins.

This paper presents the results of a thermal treatment process for magnetite nanoparticles in the temperature range of 50-500 °C. The tested magnetite nanoparticles were synthesized using three different methods that resulted in nanoparticles with different surface characteristics and crystallinity, which in turn, was reflected in their thermal durability. The particles were obtained by coprecipitation from Fe chlorides and decomposition of an Fe(acac)3 complex with and without a core-shell structure. Three types of ferrite nanoparticles were produced and their thermal stability properties were compared. In this study, two sets of unmodified magnetite nanoparticles were used where crystallinity was as determinant of the series. For the third type of particles, a Ag shell was added. By comparing the coated and uncoated particles, the influence of the metallic layer on the thermal stability of the nanoparticles was tested. Before and after heat treatment, the nanoparticles were examined using transmission electron microscopy, IR spectroscopy, differential scanning calorimetry, X-ray diffraction and Mössbauer spectroscopy. Based on the obtained results, it was observed that the fabrication methods determine, to some extent, the sensitivity of the nanoparticles to external factors.

The atomic and magnetic structure of the 1/1 Tb(14)Au(70)Si(16) quasicrystal approximant has been solved by combining x-ray and neutron diffraction data. The atomic structure is classified as a Tsai-type 1/1 approximant with certain structural deviations from the prototype structures; there are additional atomic positions in the so-called cubic interstices as well as in the cluster centers. The magnetic property and neutron diffraction measurements indicate the magnetic structure to be ferrimagnetic-like below 9 K in contrast to the related Gd(14)Au(70)Si(16) structure that is reported to be purely ferromagnetic.

Graphene nanoscrolls are Archimedean-type spirals formed by rolling single-layer graphene sheets. Their unique structure makes them conceptually interesting and understanding their formation gives important information on the manipulation and characteristics of various carbon nanostructures. Here we report a 100% efficient process to transform nitrogen-doped reduced graphene oxide sheets into homogeneous nanoscrolls by decoration with magnetic γ-Fe2O3 nanoparticles. Through a large number of control experiments, magnetic characterization of the decorated nanoparticles, and ab initio calculations, we conclude that the rolling is initiated by the strong adsorption of maghemite nanoparticles at nitrogen defects in the graphene lattice and their mutual magnetic interaction. The nanoscroll formation is fully reversible and upon removal of the maghemite nanoparticles, the nanoscrolls return to open sheets. Besides supplying information on the rolling mechanism of graphene nanoscrolls, our results also provide important information on the stabilization of iron oxide nanoparticles.

We report magnetic, dielectric, and magnetodielectric responses of the pure monoclinic bulk phase of partially disordered La2NiMnO6, exhibiting a spectrum of unusual properties and establish that this compound is an intrinsically multiglass system with a large magnetodielectric coupling (8%-20%) over a wide range of temperatures (150-300 K). Specifically, our results establish a unique way to obtain colossal magnetodielectricity, independent of any striction effects, by engineering the asymmetric hopping contribution to the dielectric constant via the tuning of the relative-spin orientations between neighboring magnetic ions in a transition-metal oxide system. We discuss the role of antisite (Ni-Mn) disorder in emergence of these unusual properties.

The complex perovskite Pb(2)CoTeO(6) (PCTO) has been prepared as polycrystalline powders by a solid state reaction route, and the crystal structure and magnetic properties have been investigated using a combination of X-ray and neutron powder diffraction, electron microscopy, dielectric, calorimetric and magnetic measurements. It was shown that at room temperature this compound adopts a trigonal perovskite structure, space group R3 (a = 5.6782(1) Å, c = 13.8552(3) Å). The compound undergoes a number of temperature-induced phase transitions and adopts four different structures in the temperature range 5-500 K: monoclinic in P2(1)/n (5 < T < 125 K, tilt system (a(+)b(-)b(-))), monoclinic in I2/m (125 < T < 210 K, tilt system (a(0)b(-)b(-))), rhombohedral in R3 (210 < T < 370 K, tilt system (a(-)a(-)a(-))), and finally cubic in Fm3m (above 370 K without any tilting). These structural phase transitions are coupled to changes in the dielectric constant and the heat capacity around 210 and 370 K. A long-range antiferromagnetically ordered state has been identified from neutron powder diffraction and magnetic studies at different temperatures. Magnetic diffraction peaks were registered below the transition at about 16 K and a possible model for the magnetic structure is proposed. Possible coexistence of long-range ordering of the electrical dipoles and the magnetic moments at low temperatures making PCTO a potential multiferroic candidate is discussed.

A reaction between nickel(II) sulfate and hydrazine in aqueous solution yields blue crystals of [Ni(6)(N(2)H(4))(6)(SO(4))(4)(OH)(2)(H(2)O)(8)](SO(4))(H(2)O)(10). The compound has been characterized by single-crystal and powder X-ray diffraction, vibrational spectroscopy, as well as variable-temperature magnetic susceptibility. This is the first reported crystal structure of the nickel(II) complex with hydrazine. The complex cation in the compound has a remarkable structure with unusual diversity of bridging groups including hydrazine molecules, sulfate ions, and hydroxo groups. Hydrazine molecules bridge nickel ions into trimers, which are further linked into hexamers through bridging sulfates. The magnetic susceptibility study of the compound reveals antiferromagnetic interaction between nickel(II) ions in the polynuclear complex.

The complex perovskite Ba(2)CoTeO(6) (BCTO) has been synthesised, and the crystal structure and magnetic properties have been investigated using a combination of X-ray and neutron powder diffraction, electron microscopy and dielectric, calorimetric and magnetic measurements. It is shown that at room temperature this compound adopts the 6L-trigonal perovskite structure, space group P3[combining macron]m (s.g. 164) (a = 5.7996(1) A, c = 14.2658(3) A). The structure comprises dimers of face-sharing octahedra as well as octahedra which share only vertices with their neighbours. Dielectric measurements indicate a diffuse transition of antiferroelectric nature near 280 K. A long-range antiferromagnetically ordered state has been identified from neutron diffraction and magnetic studies. The magnetic diffraction peaks were registered below the magnetic transition at about 15 K and a possible model for the magnetic structure is proposed. The structural and magnetic features of this compound are discussed and compared with those of other Co-based quaternary oxides adopting the perovskite structure.

We have studied alloying of the nonmagnetic spacer layer with a magnetic material as a method of tuning the interlayer coupling in magnetic multilayers. We have specifically studied the Fe/V(100) system by alloying the spacer V with various amounts of Fe. For some Fe concentrations in the spacer, it is possible to create a competition between antiferromagnetic Ruderman-Kittel-Kasuya-Yoshida exchange and direct ferromagnetic exchange coupling. The exchange coupling and transport properties for a large span of systems with different spacer concentrations and thicknesses were calculated and measured experimentally and good agreement between observations and theory was observed. A reduction in magnetoresistance of about 50% was observed close to the switchover from antiferromagnetic to ferromagnetic coupling.

We report on the experimental realization of tetragonal Fe-Co alloys as a constituent of Fe0.36Co0.64/Pt superlattices with huge perpendicular magnetocrystalline anisotropy energy, reaching 210 microeV/atom, and a saturation magnetization of 2.5 microB/atom at 40 K, in qualitative agreement with theoretical predictions. At room temperature the corresponding values and are achieved. This suggests that Fe-Co alloys with carefully chosen combinations of composition and distortion are good candidates for high-density perpendicular storage materials.

Aging in a Heisenberg-like spin glass Ag(11 at. % Mn) is investigated by measurements of the zero-field-cooled magnetic relaxation at a constant temperature after small temperature shifts absolute value of Delta T/T(g) < 0.012. A crossover from fully accumulative to nonaccumulative aging is observed, and by converting time scales to length scales using the logarithmic growth law of the droplet model, we find quantitative evidence that positive and negative temperature shifts cause an equivalent restart of aging (rejuvenation) in terms of dynamical length scales. This result supports the existence of a unique overlap length between a pair of equilibrium states in the spin-glass system.

Nonequilibrium dynamics of three-dimensional model spin glasses, the Ising system Fe0.50Mn0.50TiO3 and the Heisenberg-like system Ag(11 at % Mn), has been investigated by measurements of the isothermal time decay of the low frequency ac susceptibility after a quench from the paramagnetic to the spin-glass phase. It is found that the relaxation data measured at different temperatures can be scaled according to predictions from the droplet scaling model, provided that critical fluctuations are accounted for in the analyses.

A three-dimensional lattice of the Josephson junctions with a finite self-conductance is employed to model ceramic superconductors. By using Monte Carlo simulations it is shown that the aging disappears in the strong screening limit. In the weak screening regime, aging is present even at low temperatures. For intermediate values of the self-inductance, aging occurs in an intermediate temperature interval but is suppressed entirely at high and low temperatures. Our results are in good agreement with experiments.

The spectral and magnetic properties of iron(III) bound in the metal binding sites of human serum transferrin with oxalate or bicarbonate as synergistic anions has been studied with Mössbauer spectroscopy and electron paramagnetic resonance (EPR). The Mössbauer spectra of the iron(III) in diferric transferrin with oxalate have been described using a spin Hamiltonian with the values of the zero field splitting parameter, D = 0.55 +/- 0.05 cm-1, and the rhombicity of the crystal field, E/D = 0.045 +/- 0.005. The EPR spectrum can be described with D = 0.58 cm-1 and E/D = 0.057, using a g-strain model for the lineshape that is based on a Gaussian distribution of D and E/D with Gaussian widths sigma(D) = 0.35 cm-1 and sigma(E/D) = 0.013, respectively. The rhombicity of the iron surroundings for the transferrin-oxalate complex is almost one order of magnitude smaller than for the bicarbonate complex and the zero field splitting parameter is twice as large in the oxalate as in the bicarbonate complex. We conclude that the crystal field symmetry of the iron site is almost tetragonal in the oxalate complex but rhombohedral in the bicarbonate complex, reflecting the different geometries of the oxalate and bicarbonate coordination. The isomer shift delta = 0.56 +/- 0.01 mm s-1 and the quadrupole splitting delta EQ = 0.2 +/- 0.1 mm s-1, on the other hand, are very close to the values found for the bicarbonate complex. No differences between the Mössbauer spectra of the two iron(III) ions in diferric transferrin with oxalate were found. The homogeneity of the diferric transferrin samples was controlled by capillary zone electrophoresis in the presence of urea.