arXiv subjects

O. Gutfleisch

Publications and source records attributed to O. Gutfleisch.

13 recordsLinked to original sources

arXiv2025

Two-component anomalous Hall and Nernst effects in anisotropic Fe$_{4-x}$Ge$_x$N thin films

A series of thin films Fe$_{4-x}$Ge$_x$N (x=0-1) was fabricated onto MgO substrates by magnetron sputtering with the aim of studying the possible enhancement of the anomalous Nernst effect (ANE), envisaged based on Density Functional Theory (DFT) calculations. The Nernst and Hall effects of the series were systematically analyzed, complemented with resistivity, magnetic, electron microscopy and M\"ossbauer experiments, and DFT calculations including elastic properties. The Fe$_4$N phase crystallizes in the cubic symmetry with Pm3m space group, whereas a small tetragonal distortion is realized in for x>0.35. From the comparison of the experimental isomer shift with DFT calculations, we conclude that Ge occupies the 4b site in the tetragonal I4/mcm tructure. Ferromagnetic T$_C$ decreases rapidly from 750 K for x=0 to 100 K for x=1. The tetragonal samples with x=0.8 and 1 display two-component behavior in the Hall and Nernst effects hysteresis loops, which can be analyzed as a sum of positive and negative loops with different saturation fields. This unusual behavior is a product of a combination of several factors. (1) Co-existence of two different crystallographic orientations in the tetragonal thin film, namely with the majority of c-axis and minority of a-axis normal to the film surface. (2) Opposite sign of the anomalous Hall and Nernst effects for the direction of magnetization along the a and c-axis revealed by DFT calculation. (3) The magnetocrystalline anisotropy characterized by an easy ab-plane, which is responsible for the different saturation fields for a and c-axis. The maximum ANE was determined to be 0.9 $\mu$V/K for x=0 at room temperature, and -0.85 $\mu$V/K for x=1 at T=50 K. The rapid increase of ANE of Fe$_3$GeN from low temperatures indicates that, were it not for its low T$_C$, it could surpass ANE of Fe$_4$N.

cond-mat.mtrl-sci↗

arXiv2023

A multi-stage, first-order phase transition in LaFe11.8Si1.2: interplay between the structural, magnetic and electronic degrees of freedom

Alloys with a first-order magnetic transition are central to solid-state refrigeration technology, sensors and actuators, or spintronic devices. The discontinuous nature of the transition in these materials is a consequence of the coupling between the magnetic, electronic and structural subsystems, but in a real experiment, it is difficult to observe and analyze the simultaneous evolution of all the subsystems. As a result, it is very hard to determine the main mechanisms of the transition and purposefully develop these advanced magnetic materials. To resolve this issue, we changed the existing paradigm and conducted simultaneous measurements of the macroscopic properties - magnetization, temperature change of the sample, longitudinal and transversal magnetostrictions - to reveal the rich details of the magneto-structural, first-order transition occurring in the prototypical alloy LaFe11.8Si1.2. We complement these findings with experiments on the atomistic scale, i.e., x-ray absorption spectroscopy (XAS), x-ray magnetic circular dichroism (XMCD) and Mössbauer spectroscopy, and then combine them with first-principles calculations to reveal the full complexity and two-stage nature of the transition. This new approach can be successfully extended to a large class of advanced magnetic materials that exhibit analogous transformations.

cond-mat.mtrl-sci↗

arXiv2022

Emergence of a hidden magnetic phase in LaFe11.8Si1.2 investigated by inelastic neutron scattering as a function of field and temperature

The NaZn13 type itinerant magnet LaFe13-xSix has seen considerable interest due to its unique combination of large magnetocaloric effect and low hysteresis. Here we demonstrate, with a combination of magnetometry, bespoke microcalorimetry and inelastic neutron scattering that this is due to the presence of paramagnetic spin fluctuations, which build up as the critical point is approached. While thermal measurements show significant latent heat independent changes in the heat capacity, inelastic neutron scattering reveals the presence of broad quasielastic scattering that persists above Tc, in addition to a finite Q quasielastic peak at Q=0.52 A$^{-1}$ (close to a 100 Bragg reflection in this system at Q = 0.54 A$^{-1}$). This finite Q quasielastic peak appears only in the paramagnetic state and when in proximity to the itinerant metamagnetic transition. We associate these observations with a hidden competing phase and spin fluctuations close to the transition temperature and magnetic field, that persist across the magnetic transition.

cond-mat.str-el↗

arXiv2021

Influence of the martensitic transformation kinetics on the magnetocaloric effect in Ni-Mn-In

The inverse magnetocaloric effect (MCE) in Ni-Mn-based Heusler compounds occurs during the magnetostructural transition between low-temperature, low-magnetization martensite and high-temperature, high-magnetization austenite. In this study, we analyze the metamagnetic transformation of a $Ni_{49.8}Mn_{35}In_{15.2}$ compound by simultaneous adiabatic temperature change and strain measurements in pulsed magnetic fields up to 10 T. We observe an adiabatic temperature change of -10 K and a strain of -0.22 % when the reverse martensitic transition is fully induced at a starting temperature of 285 K. By a variation of the magnetic field-sweep rates between 316 Ts$^{-1}$, 865 Ts$^{-1}$ and 1850 Ts$^{-1}$, the transitional dynamics of the reverse martensitic transformation have been investigated. Our experiments reveal an apparent delay upon the end of the reverse martensitic transformation at field rates exceeding 865 Ts$^{-1}$ which is related to the annihilation of retained martensite. As a consequence, the field hysteresis increases and higher fields are required to saturate the transition. In contrast, no time-dependent effects on the onset of the reverse martensitic transformation were observed in the studied field-sweep range. Our results demonstrate that kinetic effects in Heusler compounds strongly affect the magnetic cooling cycle, especially when utilising a multicaloric "exploiting-hysteresis cycle" where high magnetic field-sweep rates are employed.

cond-mat.mtrl-sci↗

arXiv2019

An accelerating approach of designing ferromagnetic materials via machine learning modeling of magnetic ground state and Curie temperature

Magnetic materials have a plethora of applications ranging from informatics to energy harvesting and conversion. However, such functionalities are limited by the magnetic ordering temperature. In this work, we performed machine learning on the magnetic ground state and the Curie temperature (TC), using generic chemical and crystal structural descriptors. Based on a database of 2805 known intermetallic compounds, a random forest model is trained to classify ferromagnetic and antiferromagnetic compounds and to do regression on the TC for the ferromagnets. The resulting accuracy is about 86% for classification and 92% for regression (with a mean absolute error of 58K). Composition based features are sufficient for both classification and regression, whereas structural descriptors improve the performance. Finally, we predict the magnetic ordering and TC for all the intermetallic magnetic materials in the Materials Project. Our work paves the way to accelerate the development of magnetic materials for technological applications.

cond-mat.mtrl-sci↗

arXiv2019

Dynamics of the magnetoelastic phase transition and adiabatic temperature change in Mn1.3Fe0.7P0.5Si0.55

The adiabatic temperature change DTad of a Mn1.3Fe0.7P0.5Si0.55 Fe2P-type alloy was measured under different magnetic field-sweep rates from 0.93 Ts-1 to 2870 Ts-1. We find a field-sweep-rate independent magnetocaloric effect due to a partial alignment of magnetic moments in the paramagnetic region overlapping with the magnetocaloric effect of the first-order phase transition. Additionally, the first-order phase transition is not completed even in fields up to 20 T leading to a non-saturating behavior of DTad. Measurements in different pulsed fields reveal that the first-order phase transition cannot follow the fast field changes as previously assumed, resulting in a distinct field-dependent hysteresis in DTad.

physics.app-ph↗

arXiv2019

Pele's hairs and exotic multiply twinned graphite closed-shell microcrystals in meteoritic dust of Chelyabinsk superbolide

When a space body enters Earth's atmosphere, its surface is exposed to high pressure and temperatures. The airflow tears off small droplets from the meteoroid forming a cloud of meteorite dust. Can new materials be synthesized in these unique conditions (high temperature, pressure, gaseous atmosphere, catalysts)? As a rule, meteoritic dust dissipates in the atmosphere without a trace or is mixed with terrestrial soil. The Chelyabinsk superbolide, the biggest in the 21st century, which exploded on February 15, 2013 above snowy fields of the Southern Urals, was an exception. Two new types of materials were found during an in-depth study: thread-like structures that were not previously associated with meteorite falls and unique carbon crystals with a size of several micrometers that were not observed before. The nature of formation of thread-like structures is fully similar to the nature of formation of Pele's hair during eruptions of terrestrial volcanos. Multiple twin growth mechanism of formation of closed shell graphite microcrystals was proposed based on DFT and classical/ab initio MD simulations. It was found that among several possible embryo carbon nanoclusters the C60 fullerene and polyhexacyclooctadecane -C18H12- may be the main suspects responsible for the formation of closed shell quasi-spherical and hexagonal rod graphite microcrystals.

cond-mat.mtrl-sci↗

arXiv2019

Database of novel magnetic materials for high-performance permanent magnet development

This paper describes the open Novamag database that has been developed for the design of novel Rare-Earth free/lean permanent magnets. The database software technologies, its friendly graphical user interface, advanced search tools and available data are explained in detail. Following the philosophy and standards of Materials Genome Initiative, it contains significant results of novel magnetic phases with high magnetocrystalline anisotropy obtained by three computational high-throughput screening approaches based on a crystal structure prediction method using an Adaptive Genetic Algorithm, tetragonally distortion of cubic phases and tuning known phases by doping. Additionally, it also includes theoretical and experimental data about fundamental magnetic material properties such as magnetic moments, magnetocrystalline anisotropy energy, exchange parameters, Curie temperature, domain wall width, exchange stiffness, coercivity and maximum energy product, that can be used in the study and design of new promising high-performance Rare-Earth free/lean permanent magnets. The results therein contained might provide some insights into the ongoing debate about the theoretical performance limits beyond Rare-Earth based magnets. Finally, some general strategies are discussed to design possible experimental routes for exploring most promising theoretical novel materials found in the database.

cond-mat.mtrl-sci↗

arXiv2017

Moment-volume coupling in La(Fe$_{1-x}$Si$_x$)$_{13}$

We investigate the origin of the volume change and magnetoelastic interaction observed at the magnetic first-order transition in the magnetocaloric system La(Fe$_{1-x}$Si$_x$)$_{13}$ by means of first-principles calculations combined with the fixed-spin moment approach. We find that the volume of the system varies with the square of the average local Fe moment, which is significantly smaller in the spin disordered configurations compared to the ferromagnetic ground state. The vibrational density of states obtained for a hypothetical ferromagnetic state with artificially reduced spin-moments compared to a nuclear inelastic X-ray scattering measurement directly above the phase transition reveals that the anomalous softening at the transition essentially depends on the same moment-volume coupling mechanism. In the same spirit, the dependence of average local Fe moment on the Si content can account for the occurence of first- and second-order transitions in the system.

cond-mat.mtrl-sci↗

arXiv2015

Magnetic properties of (Fe$_{1-x}$Co$_x$)$_2$B alloys and the effect of doping by 5$d$ elements

We have explored, computationally and experimentally, the magnetic properties of \fecob{} alloys. Calculations provide a good agreement with experiment in terms of the saturation magnetization and the magnetocrystalline anisotropy energy with some difficulty in describing Co$_2$B, for which it is found that both full potential effects and electron correlations treated within dynamical mean field theory are of importance for a correct description. The material exhibits a uniaxial magnetic anisotropy for a range of cobalt concentrations between $x=0.1$ and $x=0.5$. A simple model for the temperature dependence of magnetic anisotropy suggests that the complicated non-monotonous temperature behaviour is mainly due to variations in the band structure as the exchange splitting is reduced by temperature. Using density functional theory based calculations we have explored the effect of substitutional doping the transition metal sublattice by the whole range of 5$d$ transition metals and found that doping by Re or W elements should significantly enhance the magnetocrystalline anisotropy energy. Experimentally, W doping did not succeed in enhancing the magnetic anisotropy due to formation of other phases. On the other hand, doping by Ir and Re was successful and resulted in magnetic anisotropies that are in agreement with theoretical predictions. In particular, doping by 2.5~at.\% of Re on the Fe/Co site shows a magnetocrystalline anisotropy energy which is increased by 50\% compared to its parent (Fe$_{0.7}$Co$_{0.3}$)$_2$B compound, making this system interesting, for example, in the context of permanent magnet replacement materials or in other areas where a large magnetic anisotropy is of importance.

cond-mat.mtrl-sci↗

arXiv2014

Element-resolved thermodynamics of magnetocaloric LaFe$_{13-x}$Si$_x$

By combination of two independent approaches, nuclear resonant inelastic X-ray scattering and first-principles calculations in the framework of density functional theory, we determine the element-resolved vibrational density of states in the ferromagnetic low temperature and paramagnetic high temperature phase of LaFe$_{13-x}$Si$_x$. This allows us to derive the lattice and electronic contribution to the entropy change at the first-order phase transformation, which are both of considerable magnitude. The change in lattice entropy is dominated by magneto-elastic softening, which originates from the itinerant electron metamagnetism associated with Fe. This counteracts the large volume change at the transition and leads to an unexpected, cooperative behavior of magnetic, vibrational and electronic entropy change, which is responsible for the large magneto- and barocaloric effect observed for this material.

cond-mat.mtrl-sci↗

arXiv2002

Comparative Study of Dense Bulk MgB$_2$ Materials Prepared by Different Methods

We report on the results of a comparative investigation of highly dense bulk MgB$_2$ samples prepared by three methods: (i) hot deformation; (ii) high pressure sintering; and (iii) mechanical alloying of Mg and B powders with subsequent hot compaction. All types of samples were studied by ac-susceptibility, dc-magnetization and resistivity measurements in magnetic fields up to $μ_0H=160$ kOe. A small but distinct anisotropy of the upper critical field $H_{c2}^{a,b}/H_{c2}^{c}\sim1.2$ connected with some texture of MgB$_2$ grains was found for the hot deformed samples. The samples prepared by high pressure sintering as well as by mechanical alloying show improved superconducting properties, including high upper critical fields $H_{c2}$ ($μ_0H_{c2}(0)\sim23$ T), irreversibility fields $H_{irr}$ which are strongly shifted towards higher values $H_{irr}(T)\sim0.8H_{c2}(T)$ and high critical current $J_c$ ($J_c=10^5$ A/cm$^2$ at 20 K and 1 T).

cond-mat.supr-con↗

arXiv2001

Fully dense MgB_2 superconductor textured by hot deformation

Bulk textured MgB_2 material of nearly full density showing a weak c-axis alignment of the hexagonal MgB_2 grains parallel to the pressure direction was obtained by hot deformation of a stoichiometric MgB_2 pellet prepared by a gas-solid reaction. The texture of the material was verified by comparing the x-ray diffraction patterns of the hot deformed material with isotropic MgB_2 powder. A small, but distinct anisotropy of the upper critical field up to Hc2^{a,b}/Hc2^{c}~1.2 depending on degree of texture was found by resistance and susceptibility measurements. No anisotropy of the critical current density determined from magnetization measurements was found for the textured material.

cond-mat.supr-con↗