Magnetic and Ferroic Materials

Nanoscale Electrodeposition and Magnetoionics

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Magnetic Materials

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Magnetic Microstructures

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Functional Ferroic Materials, Films, and Devices

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Nanoscale Electrodeposition and Magnetoionics

Karin Leistner and her co-worker seek to discover novel electrochemical approaches to tune functional properties of nanoscale materials. Aspects of magnetism, electrochemistry and materials science are strongly cross-linked and advanced in situ measurement techniques are developed. One focus lies on magneto-ionic effects which are based on reversible ionic motion and electrochemical reactions. These approaches enable a non-volatile low-voltage control of magnetism up to ON/OFF switching at room temperature and are therefore highly attractive for energy-efficient magnetic actuation, spintronics, and magnetophoretic devices. The materials are based on Fe, Co, FeNi and FePt nanostructures as well as Co/Ni multilayers polarized in liquid electrolyte. In situ methods based on the anomalous Hall effect, ferromagnetic resonance and Kerr microscopy measurements allow us to probe nanomagnetism in electrochemical environment. A second focus lies on the nanoelectrodeposition of magnetic elements and alloys (Fe, Co, FePt) and the understanding of electrode processes during the nucleation stage and epitaxial growth mechanisms. For example, epitaxial Fe nanocuboids are achieved, which are ideal to study the shape- and size-dependent evolution of magnetism in reduced dimension. Collaborators include the Simon Fraser University (Canada), the Massachusetts Institute of Technology (USA), the University of Kassel, and the TU Vienna.

Contact

Dr. Karin Leistner

Head of Junior Research Group  "Nanoscale Electrodeposition and Magnetoionics"

Room B3E.12
Phone: +49 351 4659 159
FAX: +49 351 4659 541

E-mail



Magnetic Materials

The group of Tom Woodcock focusses on fundamental and applied aspects of novel magnetic materials, which are needed for application in highly efficient electric motors and generators. Our current interest is in rare-earth-free permanent magnets based on Mn-Al-C alloys. The performance of magnetic materials depends not only on their intrinsic magnetic properties but also on the microstructure over length scales from pm to cm. Understanding and controlling the complex interactions which arise is highly challenging and requires both high quality materials synthesis and state-of-the-art materials characterisation. We synthesize nano- and microcrystalline materials using a variety of melting, powder metallurgy and deformation techniques. We carry out materials characterisation using scanning and transmission electron microscopy (SEM and TEM), electron backscatter diffraction (EBSD), x-ray diffraction and a variety of physical properties measurement techniques including at applied magnetic fields of up to 14 T.

Contact

Dr. Thomas G. Woodcock

Head of Research Group "Magnetic Materials"
Room B1E.11
Phone: +49 351 4659 221
E-mail

Recent Highlights

F. Bittner et al., Journal of Alloys and Compounds 727 (2017) 1095-1099
URL

As τ-MnAl is a thermodynamically metastable phase, it tends to decompose into the equilibrium phases at elevated temperatures. This restricts the kind of processing which can be carried out. Preventing the decomposition of τ is therefore a critical factor in developing MnAl magnets. Here, the preferential nucleation of the equilibrium phases at general grain boundaries rather than other interfacial types is shown using electron backscatter diffraction measurements. This explains the higher resistance to decomposition of materials which contain low fractions of general grain boundaries.

A. Chirkova et al., Acta Materialia 131 (2017) 31-38
URL

FeRh alloys undergo a magnetic transition from the antiferromagnetic state to the ferromagnetic state. The transition temperature has been shown to vary with prior heat treatment but the reason for this was unknown. In this paper, microstructural investigations showed that heat treaments led to different number density, size, shape and distribution of the secondary fcc phase. Finite element models indicated that stress fields from the secondary phase grains could overlap, thus influencing the transition temperature of the main phase through the well-known effect of pressure.

T. Mix et al., Acta Materialia 128 (2017) 160-165
URL

Two different L10 phases can be made to coexist in alloys of the form Mn55Al45-xGax with 5 < x < 9. One appears to be thermodynamically stable, like binary MnGa, and the other is metastable, like binary MnAl, but in the ternary alloys, both phases contain only a few atomic percent of Ga. The thermodynamically stable L10 phase does not undergo a phase transformation at temperatures up to at least 700°C. These results enable longer processing times at higher temperatures thus facilitating the development of rare earth free MnAl-based magnets which are capable of providing a sustainable alternative to certain types of Nd-Fe-B.

F. Bittner et al., Journal of Alloys and Compounds 704 (2017) 528-536
URL

Swaged bars of τ-MnAl show a highly twinned microstructure and a high coercivity of about 0.3 T. On annealing this material, the microstructure does not visibly change but the coercivity decreases dramatically. The sharpness of EBSD patterns is affected by the local density of dislocations. EBSD pattern quality results implied that the dislocation density was much higher in the as-swaged state. It was concluded that dislocations can act as pinning centres for domain walls in MnAl and this was supported by the magnetic new curve.

F. Bittner et al., Acta Materialia 101 (2015) 48-54
URL

Electron backscattered diffraction was used to identify three distinct interfaces which are present in L10 ordered MnAl-C. They are denoted as true twins, order twins and pseudo twins and can be described by different rotations about the normal to {111}. True twins were often observed in this material but the other two interfaces are heretofore unknown in MnAl-C. The frequency of the different interfaces was very sensitive to the sample state. Hot extrusion led to a clear preference of true twins while order twins and pseudo twins tend to disappear. A mechanism for the formation of the two yet unknown interfaces is proposed.



Analysis of Magnetic Microstructure

Our research touches the rich world of magnetic microstructure or magnetic domains, extending from the nano-world to visible dimensions. The subject, which might be called „mesomagnetism“, forms the link between atomic foundations and technical applications of magnetic materials, ranging from computer storage systems to the cores of electrical machinery, and including novel research fields like spintronics and spinorbitronics. In collaboration with technology groups we are contributing to a fundamental understanding of magnetic domains and magnetization processes in all kinds of ferro-, ferri- and antiferromagnetic materials of current interest, mainly based on their experimental analysis by advanced magneto-optic imaging- and magnetometry techniques.

Contact

Prof. Dr. Rudolf Schäfer

Head of Department "Magnetic Microstructures"
Room A3E.06.3
Phone: +49 351 4659 223
E-mail

Dr. Ivan Soldatov

Room A1E.16
Phone: +49 351 4659 340
E-mail

Books



Functional Ferroic Materials, Films, and Devices

Ferroic materials comprise ferromagnetic, ferroelastic and ferroelectric materials. These functional materials react to external stimuli like temperature, magnetic or electric fields, and stress, which makes new functionalities possible. We cover the complete range of current scientific question, from fundamental aspects on the underlying principle, preparation of better materials to the implementation in novel devices and examine the following ferroic materials: We analyze (magnetic) shape memory alloys films, which are suitable for microactuators and use epitaxial films as a model system to understand the formation of the martensitic microstructure. To achieve a more efficient refrigeration, our research covers magnetocaloric films and multicaloric effects, which occur when straining magnetocaloric films by ferroelectric substrates. As an additional energy material, we examine thermomagnetic materials and their application in thermomagnetic generators and microsystems, which represents a promising approach for the conversion of low temperature waste heat to electricity.

News & Highlights

Energy harvesting near room temperature using a thermomagnetic generator with a pretzel-like magnetic flux topology

Anja Waske, Daniel Dzekan, Kai Sellschopp, Dietmar Berger, Alexander Stork, Kornelius Nielsch & Sebastian Fähler
Nature Energy 4, pages 68–74 (2019)

To date, there are very few technologies available for the conversion of low-temperature waste heat into electricity. Thermomagnetic generators are one approach proposed more than a century ago. Such devices are based on a cyclic change of magnetization with temperature. This switches a magnetic flux and, according to Faraday’s law, induces a voltage. Here we demonstrate that guiding the magnetic flux with an appropriate topology of the magnetic circuit improves the performance of thermomagnetic generators by orders of magnitude. Through a combination of experiments and simulations, we show that a pretzel-like topology results in a sign reversal of the magnetic flux. This avoids the drawbacks of previous designs, namely, magnetic stray fields, hysteresis and complex geometries of the thermomagnetic material. Our demonstrator, which is based on magnetocaloric plates, illustrates that this solid-state energy conversion technology presents a key step towards becoming competitive with thermoelectrics for energy harvesting near room temperature.

Caloric effects in ferroic materials

Sebastian Fähler & Vitalij K. Pecharsky
MRS Bulletin 43(4), pages 264-268 (2018)

The fundamentals and applications of ferroic materials—ferromagnetic, ferroelectric, and ferroelastic—are common subjects discussed in just about every graduate course related to functional materials. Looking beyond today’s traditional uses, such as in permanent magnets, capacitors, and shape-memory alloys, there are worthwhile and interesting questions common to the caloric properties of these ferroic materials. Can ferroic materials be used in a cooling cycle? Why are these materials susceptible to external fields? Which combination of properties is required to make some of them suitable for efficient cooling and heat pumping? We address these questions in this introduction to ferroic cooling, which comprises magnetocaloric, electrocaloric, elastocaloric and barocaloric approaches and combinations thereof (i.e., multicalorics). These are addressed in greater detail in the articles in this issue.

Modulations in martensitic Heusler alloys originate from nanotwin ordering

Markus E. Gruner, Robert Niemann, Peter Entel, Rossitza Pentcheva, Ulrich K. Rössler, Kornelius Nielsch & Sebastian Fähler
Sci. Rep. 8, page 8489 (2018)

Heusler alloys exhibiting magnetic and martensitic transitions enable applications like magnetocaloric refrigeration and actuation based on the magnetic shape memory effect. Their outstanding functional properties depend on low hysteresis losses and low actuation fields. These are only achieved if the atomic positions deviate from a tetragonal lattice by periodic displacements. The origin of the so-called modulated structures is the subject of much controversy: They are either explained by phonon softening or adaptive nanotwinning. Here we used large-scale density functional theory calculations on the Ni2MnGa prototype system to demonstrate interaction energy between twin boundaries. Minimizing the interaction energy resulted in the experimentally observed ordered modulations at the atomic scale, it explained that a/b twin boundaries are stacking faults at the mesoscale, and contributed to the macroscopic hysteresis losses. Furthermore, we found that phonon softening paves the transformation path towards the nanotwinned martensite state. This unified both opposing concepts to explain modulated martensite.

Reversible tuning of magnetocaloric Ni-Mn-Ga-Co films on ferroelectric PMN-PT substrates

Benjamin Schleicher, Robert Niemann, Stefan Schwabe, Ruben Hühne, Ludwig Schultz, Kornelius Nielsch & Sebastian Fähler
Sci. Rep. 7, page 14462 (2017)

Tuning functional properties of thin caloric films by mechanical stress is currently of high interest. In particular, a controllable magnetisation or transition temperature is desired for improved usability in magnetocaloric devices. Here, we present results of epitaxial magnetocaloric Ni-Mn-Ga-Co thin films on ferroelectric Pb(Mg1/3Nb2/3)0.72Ti0.28O3 (PMN-PT) substrates. Utilizing X-ray diffraction measurements, we demonstrate that the strain induced in the substrate by application of an electric field can be transferred to the thin film, resulting in a change of the lattice parameters. We examined the consequences of this strain on the magnetic properties of the thin film by temperature- and electric field-dependent measurements. We did not observe a change of martensitic transformation temperature but a reversible change of magnetisation within the austenitic state, which we attribute to the intrinsic magnetic instability of this metamagnetic Heusler alloy. We demonstrate an electric field-controlled entropy change of about 31 % of the magnetocaloric effect - without any hysteresis.

Current Projects

  • Thermal Micro Energy Harvesting by Thermomagnetic Film Actuation
    Manfred Kohl, Sebastian Fähler (DFG, FA 453/14)
    This project on “Thermal micro energy harvesting by thermomagnetic film actuation” investigates a novel approach to generate electrical energy from thermal energy on the miniature scale. It expands a precursor project at KIT, in which thermomagnetic generators (TMGs) have been developed, reaching average power densities of the active material of 118 mW cm-3 and 5% of Carnot efficiency. These specifications already compete with the best thermoelectric generators at the length scale of a centimetre and below. The current project addresses the key characteristics of a TMG: (1) Expansion of the usable temperature range to 30–100°C, (2) increase of electrical power, and (3) improvement of thermodynamic efficiency. As the performance of miniaturized TMGs is intimately connected with the functional properties of the thermomagnetic films used, this joint proposal brings together the complementary competence on microsystem engineering of KIT and thermomagnetic materials science of IFW.For optimization of TMG characteristics (1)-(3), the thermomagnetic properties of Ni-Mn-based Heusler and Ga-based films (transition temperatures, temperature-dependent change of magnetization, dM/dT, hysteresis) will be tailored by varying composition and degree of order. The design of the TMGs will be optimized by improving heat transfer, enhancing magnetic field gradient, as well as tuning mechanical resonance. In particular, for the improvement of heat transfer micromachined films will be applied, containing trenches filled by Cu. The scaling properties of TMG characteristics will be investigated experimentally, as well as by lumped element modelling. Based on the optimum scaling of a single TMG, distributed systems of 1D and 2D arrays of TMGs will be developed in order to bring the total power in line with the practical needs of IoT and industry4.0.

  • Martensitic phase transformation and twinning in epitaxially grown Nickel Titanium films
    Martin F.-X. Wagner, Sebastian Fähler (DFG, FA 453/13)
    In this research project we study epitaxially grown NiTi shape memory alloy films. These thin films (with thicknesses ranging from about 100 nm to several microns) are used as a model system for highly precise, fundamental investigations on martensitic transformations, for instance to analyze on several length scales the self-similar martensitic microstructures in NiTi. Most importantly, we will consider the key question whether the morphology of martensitic microstructures in NiTi is determined by thermodynamic equilibrium processes or by the most easily accessible transformation paths. The planned experimental work considers epitaxial growth of NiTi films on different MgO and Al2O3 substrates. Moreover, we use X-ray diffraction, atomic force microscopy and electron microscopy methods to analyze the twinned microstructures and the corresponding textures of NiTi martensites. In in-situ investigations, the martensitic phase transition is documented by atomic force microscopy measurements during cooling, with a particular focus on nucleation mechanisms. The stress-induced transformation is triggered using nanoindentation and small-scale tensile testing of free-standing thin films; the activated twinning systems are analyzed by means of micromechanical and continuum mechanical calculations considering elastic anisotropy of both high and low temperature phases. The experimental and theoretical results of our investigations on the well-defined model system will allow to describe formation of martensitic microstructures in NiTi across several relevant length-scales. The effect of different twin boundary energies on the formation of hierarchically structured martensites will be considered, and a comparison with the multi-step nucleation model, where the kinetics of the phase transition is determined by the pathway with the lowest energy barrier, will be performed.

  • Understanding magnetocaloric and electrocaloric effects using epitaxial films
    Sebastian Fähler, Ruben Hühne (DFG FA 453/11), within SPP 1599
    There is a need for more energy-efficient refrigeration to reduce the environmental impact of todays lifestyle. Solid state refrigeration based on diffusionless transformation is a promising solution. Within our joint project we focus on materials exhibiting electrocaloric or magnetocaloric effects, i.e. where the application of an electric or magnetic field leads to a temperature change. In shape of thin films such materials might be used for on-chip ferroic cooling in microelectronics or micromechanical devices. The main goal of our experimental project is to understand ferroic cooling and in particular hysteresis losses on a microstructural level. As a suitable model system we use epitaxially grown films, which enable detailed static and dynamic studies. This package project combines expertise on both, magnetocaloric films and electrocaloric epitaxial films. We aim to describe the local structure with an adaptive concept, which we already successfully applied for isostructural magnetic shape memory alloys. We will expand this concept for the description of hysteretic losses during field cycling as it is postulated that such losses are closely connected to coarsening processes in the martensitic microstructure. In particular, the phase transformation, which leads to the caloric effects, will be studied with advanced local as well with integral probes in close collaboration with other participants in the SPP. Epitaxial heterostructures will be used to tune the strain in these materials, which allows modifying caloric properties. Similar approaches will be utilized to study multicaloric effects in heterostructures. From the direct comparison of electro- and magnetocaloric materials within this package project we expect a unified description of the underlying processes during ferroic cooling. Our fundamental studies will be accompanied by indirect and direct measurements to quantify the temperature change during a cooling cycle. The results of our fundamental investigations will enable us to identify the key parameters for more efficient ferroic cooling, which will be the basis for a further optimization of materials and device structures for potential applications.  

  • Coordination of SPP 1599 FerroicCooling
    S. Fähler (DFG FA 453/10), within SPP 1599 FerroicCooling
    This project comprises the coordination of the priority program SPP 1599 FerroicCooling. It is intended to support the organisation of colloquiums and focus meetings. The interdisciplinary questions require the collaboration of material scientists, engineers, mathematicians and physicists. By regular colloquiums of all participants every year a coherent exchange of knowledge is obtained. Additionally three focus meetings per year will accelerate the exchange of know-how on specific topics. Due to the application relevant topic of this SPP, interested persons from industry are invited to these meetings. To establish an international network, the collaboration and exchange of scientists with partners abroad is supported. Ferroic cooling comprises various cooling schemes and even more materials. However, neither schemes nor materials can be compared today and evaluated with respect to their application potential. By a cross-project comparison of materials, methods and devices we intend to reach generally accepted criteria.In addition this coordinator project includes a Mercator fellowship to continue benefiting from the intense collaboration with a senior scientist as well as start-up funding for early career scientists.