arXiv subjects

Oliver Gutfleisch

Publications and source records attributed to Oliver Gutfleisch.

70 records · Page 4Linked to original sources

arXiv2019

Designing rare-earth free permanent magnets in Heusler alloys via interstitial doping

Based on high-throughput density functional theory calculations, we investigated the effects of light interstitial H, B, C, and N atoms on the magnetic properties of cubic Heusler alloys, with the aim to design new rare-earth free permanent magnets. It is observed that the interstitial atoms induce significant tetragonal distortions, leading to 32 candidates with large ($>$ 0.4 MJ/m$^3$) uniaxial magneto-crystalline anisotropy energies (MAEs) and 10 cases with large in-plane MAEs. Detailed analysis following the the perturbation theory and chemical bonding reveals the strong MAE originates from the local crystalline distortions and thus the changes of the chemical bonding around the interstitials. This provides a valuable way to tailor the MAEs to obtain competitive permanent magnets, filling the gap between high performance Sm-Co/Nd-Fe-B and widely used ferrite/AlNiCo materials.

cond-mat.mtrl-sci↗

arXiv2019

Calculating temperature-dependent properties of Nd$_2$Fe$_{14}$B permanent magnets by atomistic spin model simulations

Temperature-dependent magnetic properties of Nd$_2$Fe$_{14}$B permanent magnets, i.e., saturation magnetization $M_\text{s}(T)$, effective magnetic anisotropy constants $K_i^\text{eff}(T)$ ($i=1,2,3$), domain wall width $δ_w(T)$, and exchange stiffness constant $A_\text{e}(T)$, are calculated by using \textit{ab-initio} informed atomistic spin model simulations. We construct the atomistic spin model Hamiltonian for Nd$_2$Fe$_{14}$B by using the Heisenberg exchange of Fe$-$Fe and Fe$-$Nd atomic pairs, the uniaxial single-ion anisotropy of Fe atoms, and the crystal-field energy of Nd ions which is approximately expanded into an energy formula featured by second, fourth, and sixth-order phenomenological anisotropy constants. After applying a temperature rescaling strategy, we show that the calculated Curie temperature, spin-reorientation phenomenon, $M_\text{s}(T)$, $δ_w(T)$, and $K_i^\text{eff}(T)$ agree well with the experimental results. $A_\text{e}(T)$ is estimated through a general continuum description of the domain wall profile by mapping atomistic magnetic moments to the macroscopic magnetization. $A_\text{e}$ is found to decrease more slowly than $K_1^\text{eff}$ with increasing temperature, and approximately scale with normalized magnetization as $A_\text{e}(T) \sim m^{1.2}$. This work provokes a scale bridge between \textit{ab-initio} calculations and temperature-dependent micromagnetic simulations of Nd-Fe-B permanent magnets.

cond-mat.mtrl-sci↗

arXiv2019

Computational study on microstructure evolution and magnetic property of laser additively manufactured magnetic materials

Additive manufacturing (AM) offers an unprecedented opportunity for the quick production of complex shaped parts directly from a powder precursor. But its application to functional materials in general and magnetic materials in particular is still at the very beginning. Here we present the first attempt to computationally study the microstructure evolution and magnetic properties of magnetic materials (e.g. Fe-Ni alloys) processed by selective laser melting (SLM). SLM process induced thermal history and thus the residual stress distribution in Fe-Ni alloys are calculated by finite element analysis (FEA). The evolution and distribution of the $γ$-Fe-Ni and FeNi$_3$ phase fractions were predicted by using the temperature information from FEA and the output from CALculation of PHAse Diagrams (CALPHAD). Based on the relation between residual stress and magnetoelastic energy, magnetic properties of SLM processed Fe-Ni alloys (magnetic coercivity, remanent magnetization, and magnetic domain structure) are examined by micromagnetic simulations. The calculated coercivity is found to be in line with the experimentally measured values of SLM-processed Fe-Ni alloys. This computation study demonstrates a feasible approach for the simulation of additively manufactured magnetic materials by integrating FEA, CALPHAD, and micromagnetics.

cond-mat.mtrl-sci↗

arXiv2018

Thermoelectric determination of electronic entropy change in Ni-doped FeRh

The net entropy change corresponding to the charge carriers in a Ni-doped FeRh bulk polycrystal was experimentally evaluated in a single sample using low temperature heat capacity experiments with applied magnetic field, and using Seebeck effect and Hall coefficient measurements at high temperatures across the first order transition. From the heat capacity data a value for the electronic entropy change $ΔS_{el}\approx8.9$ J\ kg$^{-1}$K$^{-1}$ was extracted, whereas a value of up to 4 J\ kg$^{-1}$K$^{-1}$ was obtained form the Seebeck coefficient. Additionally, the analysis of the Seebeck coefficient allows tracing the evolution of the electronic entropy change with applied magnetic field. An increase of the electronic entropy with increasing applied magnetic field is evidenced, as high as 10 percent at 6 T.

cond-mat.mtrl-sci↗

arXiv2018

Tuning magnetocrystalline anisotropy of Fe$_{3}$Sn by alloying

The electronic structure, magnetic properties and phase formation of hexagonal ferromagnetic Fe$_{3}$Sn-based alloys have been studied from first principles and by experiment. The pristine Fe$_{3}$Sn compound is known to fulfill all the requirements for a good permanent magnet, except for the magnetocrystalline anisotropy energy (MAE). The latter is large, but planar, i.e. the easy magnetization axis is not along the hexagonal c direction, whereas a good permanent magnet requires the MAE to be uniaxial. Here we consider Fe$_{3}$Sn$_{0.75}$M$_{0.25}$, where M= Si, P, Ga, Ge, As, Se, In, Sb, Te and Bi, and show how different dopants on the Sn sublattice affect the MAE and can alter it from planar to uniaxial. The stability of the doped Fe$_{3}$Sn phases is elucidated theoretically via the calculations of their formation enthalpies. A micromagnetic model is developed in order to estimate the energy density product (BH)max and coercive field $μ_{0}$H$_{c}$ of a potential magnet made of Fe$_{3}$Sn$_{0.75}$Sb$_{0.25}$, the most promising candidate from theoretical studies. The phase stability and magnetic properties of the Fe$_{3}$Sn compound doped with Sb and Mn has been checked experimentally on the samples synthesised using the reactive crucible melting technique as well as by solid state reaction. The Fe$_{3}$Sn-Sb compound is found to be stable when alloyed with Mn. It is shown that even small structural changes, such as a change of the c/a ratio or volume, that can be induced by, e.g., alloying with Mn, can influence anisotropy and reverse it from planar to uniaxial and back.

cond-mat.mtrl-sci↗

arXiv2017

Multiscale examination of strain effects in Nd-Fe-B permanent magnets

We have performed a combined first-principles and micromagnetic study on the strain effects in Nd-Fe-B magnets. First-principles calculations on Nd2Fe14B reveal that the magnetocrystalline anisotropy (K) is insensitive to the deformation along c axis and the ab in-plane shrinkage is responsible for the K reduction. The predicted K is more sensitive to the lattice deformation than what the previous phenomenological model suggests. The biaxial and triaxial stress states have a greater impact on K. Negative K occurs in a much wider strain range in the ab biaxial stress state. Micromagnetic simulations of Nd-Fe-B magnets using first-principles results show that a 3-4% local strain in a 2-nm-wide region near the interface around the grain boundaries and triple junctions leads to a negative local K and thus decreases the coercivity by ~60%. The local ab biaxial stress state is more likely to induce a large loss of coercivity. In addition to the local stress states and strain levels themselves, the shape of the interfaces and the intergranular phases also makes a difference in determining the coercivity. Smoothing the edge and reducing the sharp angle of the triple regions in Nd-Fe-B magnets would be favorable for a coercivity enhancement.

cond-mat.mtrl-sci↗

arXiv2016

Impact of lattice dynamics on the phase stability of metamagnetic FeRh: Bulk and thin films

We present phonon dispersions, element-resolved vibrational density of states (VDOS) and corresponding thermodynamic properties obtained by a combination of density functional theory (DFT) and nuclear resonant inelastic X-ray scattering (NRIXS) across the metamagnetic transition of B2 FeRh in the bulk material and thin epitaxial films. We see distinct differences in the VDOS of the antiferromagnetic (AF) and ferromagnetic (FM) phase which provide a microscopic proof of strong spin-phonon coupling in FeRh. The FM VDOS exhibits a particular sensitivity to the slight tetragonal distortions present in epitaxial films, which is not encountered in the AF phase. This results in a notable change in lattice entropy, which is important for the comparison between thin film and bulk results. Our calculations confirm the recently reported lattice instability in the AF phase. The imaginary frequencies at the $X$-point depend critically on the Fe magnetic moment and atomic volume. Analyzing these non vibrational modes leads to the discovery of a stable monoclinic ground state structure which is robustly predicted from DFT but not verified in our thin film experiments. Specific heat, entropy and free energy calculated within the quasiharmonic approximation suggest that the new phase is possibly suppressed because of its relatively smaller lattice entropy. In the bulk phase, lattice degrees of freedom contribute with the same sign and in similar magnitude to the isostructural AF-FM phase transition as the electronic and magnetic subsystems and therefore needs to be included in thermodynamic modeling.

cond-mat.mtrl-sci↗

arXiv2016

Mastering hysteresis in magnetocaloric materials

Hysteresis is more than just an interesting oddity, which occurs in materials with a first-order transition. It is a real obstacle on the path from existing lab-scale prototypes of magnetic refrigerators towards commercialization of this potentially disruptive cooling technology. Indeed, the reversibility of the magnetocaloric effect, being essential for magnetic heat pumps, strongly depends on the width of the thermal hysteresis and therefore it is necessary to understand the mechanisms causing hysteresis and to find solutions how to minimize losses associated with thermal hysteresis in order to maximize the efficiency of magnetic cooling devices. In this work, we discuss fundamental aspects, which can contribute to thermal hysteresis and we are developing strategies for at least partially overcoming the hysteresis problem in some selected classes of magnetocaloric materials with large application potential. Doing so, we refer to the most relevant classes of magnetic refrigerants La-Fe-Si-, Heusler- and Fe2P-type compounds.

cond-mat.mtrl-sci↗

arXiv2016

Influence of defect thickness on the angular dependence of coercivity in rare-earth permanent magnets

The coercive field and angular dependence of the coercive field of single-grain Nd$_{2}$Fe$_{14}$B permanent magnets are computed using finite element micromagnetics. It is shown that the thickness of surface defects plays a critical role in determining the reversal process. For small defect thicknesses reversal is heavily driven by nucleation, whereas with increasing defect thickness domain wall de-pinning becomes more important. This change results in an observable shift between two well-known behavioral models. A similar trend is observed in experimental measurements of bulk samples, where a Nd-Cu infiltration process has been used to enhance coercivity by modifying the grain boundaries. When account is taken of the imperfect grain alignment of real magnets, the single-grain computed results appears to closely match experimental behaviour.

cond-mat.mtrl-sci↗

arXiv2016

Multiferroic clusters: a new perspective for relaxor-type room-temperature multiferroics

Multiferroics are promising for sensor and memory applications, but despite all efforts invested in their research no single-phase material displaying both ferroelectricity and large magnetization at room-temperature has hitherto been reported. This situation has substantially been improved in the novel relaxor ferroelectric single-phase , where polar nanoregions (PNR) transform into static-PNR (SPNR) as evidenced by piezoresponse force microscopy (PFM) and simultaneously enable congruent multiferroic clusters (MFC) to emerge from inherent ferrimagnetic Bi(Fe,Co)O3 regions as verified by magnetic force microscopy (MFM) and secondary ion mass spectrometry (SIMS). On these MFC, exceptionally large direct and converse magnetoelectric coupling coefficients, at room-temperature, were measured by PFM and MFM respectively. We expect the non-ergodic relaxor properties which are governed by the Bi0.5K0.5TiO3 component to play a vital role in the strong ME coupling, by providing an electrically and mechanically flexible environment to MFC. This new class of non-ergodic relaxor multiferroics bears great potential for applications. Especially the prospect of a ME nanodot storage device seems appealing.

cond-mat.mtrl-sci↗

arXiv2014

The dynamics of spontaneous hydrogen segregation in LaFe$_{13-x}$Si$_x$H$_y$

By means of time- and temperature-dependent magnetization measurements, we demonstrate that the timescale of hydrogen diffusion in partially-hydrogenated LaFe$_{13-x}$Si$_x$H$_y$ is of the order of hours, when the material is held at temperatures close to its as-prepared Curie temperature, $T_{C0}$. The diffusion constant is estimated to be $D \approx 10^{-15}$ - $10^{-16}$ m$^2$s$^{-1}$ at room temperature. We examine the evolution of a magnetically phase-separated state upon annealing for 3 days at a range of temperatures around $T_{C0}$, and show that the thermodynamic driving force behind hydrogen diffusion and phase segregation may be attributed to the lower free energy of hydrogen interstitials in the ferromagnetic state relative to the paramagnetic state.

cond-mat.mtrl-sci↗

arXiv2014

First-principles calculation of the instability leading to giant inverse magnetocaloric efects

The structural and magnetic properties of functional Ni-Mn-Z (Z = Ga, In, Sn) Heusler alloys are studied by first-principles and Monte Carlo methods. The \textit{ab initio} calculations give a basic understanding of the underlying physics which is associated with the strong competition of ferro- and antiferromagnetic interactions with increasing chemical disorder. The resulting $d$-electron orbital dependent magnetic ordering is the driving mechanism of magnetostructural instability which is accompanied by a drop of magnetization governing the size of the magnetocaloric effect. The thermodynamic properties are calculated by using the \textit{ab initio} magnetic exchange coupling constants in finite-temperature Monte Carlo simulations, which are used to accurately reproduce the experimental entropy and adiabatic temperature changes across the magnetostructural transition.

cond-mat.mtrl-sci↗

arXiv2008

Structural, magnetic and mechanical properties of 5 $μ$m thick SmCo films for use in Micro-Electro-Mechanical-Systems

5$μ$m thick SmCo films were deposited onto Si substrates using triode sputtering. A study of the influence of deposition temperature (Tdep <= 600 degrees C) on the structural, magnetic and mechanical properties has shown that optimum properties (highest degree of in-plane texture, maximum in-plane coercivity and remanence (1.3 and 0.8 T, respectively), no film peel-off) are achieved for films deposited at the relatively low temperature of 350 degrees C. This temperature is compatible with film integration into Micro-Electro-Mechanical-Systems (MEMS). The deposition rate was increased from 3.6 to 18 $μ$m/h by increasing the surface area of the target from 7 to 81 cm2. Mechanically stable films could be prepared by deposition onto pre-patterned films or deposition through holes in a mask.

cond-mat.mtrl-sci↗

arXiv2007

Effects of hydrostatic pressure on the magnetism and martensitic transition of Ni-Mn-In magnetic superelastic alloys

We report magnetization and differential thermal analysis measurements as a function of pressure accross the martensitic transition in magnetically superelastic Ni-Mn-In alloys. It is found that the properties of the martensitic transformation are significantly affected by the application of pressure. All transition temperatures shift to higher values with increasing pressure. The largest rate of temperature shift with pressure has been found for Ni$_{50}$Mn$_{34}$In$_{16}$ as a consequence of its small entropy change at the transition. Such a strong pressure dependence of the transition temperature opens up the possibility of inducing the martensitic transition by applying relatively low hydrostatic pressures.

cond-mat.mtrl-sci↗

arXiv2007

Evolution of magnetic and microstructural properties of thick sputtered NdFeB films with processing temperature

Ta (100 nm) / NdFeB (5 $μ$m) / Ta (100 nm) films have been deposited onto Si substrates using triode sputtering (deposition rate ~ 18 $μ$m/h). A 2-step procedure was used : deposition at temperatures up to 400 C followed by ex-situ annealing at higher temperatures. Post-deposition annealing temperatures above 650 C are needed to develop high values of coercivity. The duration of the annealing time is more critical in anisotropic samples deposited onto heated substrates than in isotropic samples deposited at lower temperatures. For a given set of annealing conditions (750 C/ 10'), high heating rates (≥ 2000 C / h) favour high coercivity in both isotropic and anisotropic films. The shape and size of Nd2Fe14B grains depend strongly on the heating rate.

cond-mat.mtrl-sci↗

arXiv2007

High performance hard magnetic NdFeB thick films for integration into Micro-Electro-Mechanical-Systems

5$μ$m thick NdFeB films have been sputtered onto 100 mm Si substrates using high rate sputtering (18 $μ$m/h). Films were deposited at ≤ 500 C and then annealed at 750 C for 10 minutes. While films deposited at temperatures up to 450 C have equiaxed grains, the size of which decreases with increasing deposition temperature, the films deposited at 500 C have columnar grains. The out-of-plane remanent magnetization increases with deposition temperature, reaching a maximum value of 1.4 T, while the coercivity remains constant at about 1.6 T. The maximum energy product achieved (400 kJ/m3) is comparable to that of high-quality NdFeB sintered magnets.

cond-mat.mtrl-sci↗