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    Rare-earth-free MnAl-C-Ni permanent magnets produced by extrusion of powder milled from bulk
    (Amsterdam : Elsevier, 2020) Feng, Le; Freudenberger, Jens; Mix, Torsten; Nielsch, Kornelius; Woodcock, Thomas George
    Rare-earth-free MnAl-C-Ni permanent magnets have been produced for the first time by extruding powders milled from bulk. The resulting materials, fabricated using different conditions, contained a large volume fraction (> 0.92) of the desired τ-phase. In terms of the maximum energy product, the best performance obtained for a whole, transverse section of the extruded material was (BH)max = 46 kJm−3, and was (BH)max = 49 kJm−3 for a sample taken from near the edge of this section. Analysis showed that this material was comparable to the long-established benchmark, comprising MnAl-C-based magnets extruded in industry from bulk or from gas-atomised powder. Such materials are no longer available. The microstructure of the materials produced here consisted of fine, recrystallised grains, which exhibited an <001> fibre texture with intermediate texture quality and of larger, non-recrystallised regions, which contained hierarchical twinning and a high density of defects. The volume fraction and size of the non-recrystallised regions was greatly reduced by decreasing the size of the initial powder particles. This led to a large increase in the squareness factor of the demagnetisation curve and consequently to the high (BH)max values observed.
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    Self‐Patterning of Multifunctional Heusler Membranes by Dewetting
    (Weinheim : Wiley-VCH, 2021) Lünser, Klara; Diestel, Anett; Nielsch, Kornelius; Fähler, Sebastian
    Ni-Mn-based Heusler alloys are an emerging class of materials which enable actuation by (magnetic) shape memory effects, magnetocaloric cooling, and thermomagnetic energy harvesting. Multifunctional materials have a particular advantage for miniaturization since their functionality is already built within the material. However, often complex microtechnological processing is required to bring these materials into shape. Here, self-organized formation of single crystalline membranes having arrays of rectangular holes with high aspect ratio is demonstrated. Dewetting avoids the need for complicated processing and allows to prepare freestanding Ni–Mn–Ga–Co membranes. These membranes are martensitic and magnetic, and their functional properties are not disturbed by self-patterning. Feature sizes of these membranes can be tailored by film thickness and heat treatment, and the tendencies can be explained with dewetting. As an outlook, the advantages of these multifunctional membranes for magnetocaloric and thermomagnetic microsystems are sketched. © 2021 The Authors. Advanced Materials Interfaces published by Wiley-VCH GmbH
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    Building Hierarchical Martensite
    (Weinheim : Wiley-VCH, 2020) Schwabe, Stefan; Niemann, Robert; Backen, Anja; Wolf, Daniel; Damm, Christine; Walter, Tina; Seiner, Hanuš; Heczko, Oleg; Nielsch, Kornelius; Fähler, Sebastian
    Martensitic materials show a complex, hierarchical microstructure containing structural domains separated by various types of twin boundaries. Several concepts exist to describe this microstructure on each length scale, however, there is no comprehensive approach bridging the whole range from the nano- up to the macroscopic scale. Here, it is described for a Ni-Mn-based Heusler alloy how this hierarchical microstructure is built from scratch with just one key parameter: the tetragonal distortion of the basic building block at the atomic level. Based on this initial block, five successive levels of nested building blocks are introduced. At each level, a larger building block is formed by twinning the preceding one to minimize the relevant energy contributions locally. This naturally explains the coexistence of different types of twin boundaries. The scale-bridging approach of nested building blocks is compared with experiments in real and reciprocal space. The approach of nested building blocks is versatile as it can be applied to the broad class of functional materials exhibiting diffusionless transformations. © 2020 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH
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    Thermoelectric Characterization Platform for Electrochemically Deposited Materials
    (Weinheim : Wiley-VCH Verlag GmbH & Co. KG, 2020) Barati, Vida; Garcia Fernandez, Javier; Geishendorf, Kevin; Schnatmann, Lauritz Ule; Lammel, Michaela; Kunzmann, Alexander; Pérez, Nicolás; Li, Guodong; Schierning, Gabi; Nielsch, Kornelius; Reith, Heiko
    Successful optimization of the thermoelectric (TE) performance of materials, described by the figure of merit zT, is a key enabler for its application in energy harvesting or Peltier cooling devices. While the zT value of bulk materials is accessible by a variety of commercial measurement setups, precise determination of the zT value for thin and thick films remains a great challenge. This is particularly relevant for films synthesized by electrochemical deposition, where the TE material is deposited onto an electrically conductive seed layer causing an in-plane short circuit. Therefore, a platform for full in-plane zT characterization of electrochemically deposited TE materials is developed, eliminating the impact of the electrically conducting seed layer. The characterization is done using a suspended TE material within a transport device which was prepared by photolithography in combination with chemical etching steps. An analytical model to determine the thermal conductivity is developed and the results verified using finite element simulations. Taken together, the full in-plane zT characterization provides an inevitable milestone for material optimization under realistic conditions in TE devices. © 2020 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
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    Transparent Power-Generating Windows Based on Solar-Thermal-Electric Conversion
    (Weinheim : Wiley-VCH, 2021) Zhang, Qihao; Huang, Aibin; Ai, Xin; Liao, Jincheng; Song, Qingfeng; Reith, Heiko; Cao, Xun; Fang, Yueping; Schierning, Gabi; Nielsch, Kornelius; Bai, Shengqiang; Chen, Lidong
    Integrating transparent solar-harvesting systems into windows can provide renewable on-site energy supply without altering building aesthetics or imposing further design constraints. Transparent photovoltaics have shown great potential, but the increased transparency comes at the expense of reduced power-conversion efficiency. Here, a new technology that overcomes this limitation by combining solar-thermal-electric conversion with a material's wavelength-selective absorption is presented. A wavelength-selective film consisting of Cs0.33WO3 and resin facilitates high visible-light transmittance (up to 88%) and outstanding ultraviolet and infrared absorbance, thereby converting absorbed light into heat without sacrificing transparency. A prototype that couples the film with thermoelectric power generation produces an extraordinary output voltage of ≈4 V within an area of 0.01 m2 exposed to sunshine. Further optimization design and experimental verification demonstrate high conversion efficiency comparable to state-of-the-art transparent photovoltaics, enriching the library of on-site energy-saving and transparent power generation.
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    Voltage‐Controlled Deblocking of Magnetization Reversal in Thin Films by Tunable Domain Wall Interactions and Pinning Sites
    (Hoboken, NJ : Wiley, 2020) Zehner, Jonas; Soldatov, Ivan; Schneider, Sebastian; Heller, René; Khojasteh, Nasrin B.; Schiemenez, Sandra; Fähler, Sebastian; Nielsch, Kornelius; Schäfer, Rudolf; Leistner, Karin
    High energy efficiency of magnetic devices is crucial for applications such as data storage, computation, and actuation. Redox‐based (magneto‐ionic) voltage control of magnetism is a promising room‐temperature pathway to improve energy efficiency. However, for ferromagnetic metals, the magneto‐ionic effects studied so far require ultrathin films with tunable perpendicular magnetic anisotropy or nanoporous structures for appreciable effects. This paper reports a fully reversible, low voltage‐induced collapse of coercivity and remanence by redox reactions in iron oxide/iron films with uniaxial in‐plane anisotropy. In the initial iron oxide/iron films, Néel wall interactions stabilize a blocked state with high coercivity. During the voltage‐triggered reduction of the iron oxide layer, in situ Kerr microscopy reveals inverse changes of coercivity and anisotropy, and a coarsening of the magnetic microstructure. These results confirm a magneto‐ionic deblocking mechanism, which relies on changes of the Néel wall interactions, and of the microstructural domain‐wall‐pinning sites. With this approach, voltage‐controlled 180° magnetization switching with high energy‐efficiency is achieved. It opens up possibilities for developing magnetic devices programmable by ultralow power and for the reversible tuning of defect‐controlled materials in general.
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    Current State-of-the-Art in the Interface/Surface Modification of Thermoelectric Materials
    (Weinheim : Wiley-VCH, 2021) He, Shiyang; Lehmann, Sebastian; Bahrami, Amin; Nielsch, Kornelius
    Thermoelectric (TE) materials are prominent candidates for energy converting applications due to their excellent performance and reliability. Extensive efforts for improving their efficiency in single-/multi-phase composites comprising nano/micro-scale second phases are being made. The artificial decoration of second phases into the thermoelectric matrix in multi-phase composites, which is distinguished from the second-phase precipitation occurring during the thermally equilibrated synthesis of TE materials, can effectively enhance their performance. Theoretically, the interfacial manipulation of phase boundaries can be extended to a wide range of materials. High interface densities decrease thermal conductivity when nano/micro-scale grain boundaries are obtained and certain electronic structure modifications may increase the power factor of TE materials. Based on the distribution of second phases on the interface boundaries, the strategies can be divided into discontinuous and continuous interfacial modifications. The discontinuous interfacial modifications section in this review discusses five parts chosen according to their dispersion forms, including metals, oxides, semiconductors, carbonic compounds, and MXenes. Alternatively, gas- and solution-phase process techniques are adopted for realizing continuous surface changes, like the core–shell structure. This review offers a detailed analysis of the current state-of-the-art in the field, while identifying possibilities and obstacles for improving the performance of TE materials.
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    Control of Positive and Negative Magnetoresistance in Iron Oxide : Iron Nanocomposite Thin Films for Tunable Magnetoelectric Nanodevices
    (2020) Nichterwitz, Martin; Honnali, Shashank; Zehner, Jonas; Schneider, Sebastian; Pohl, Darius; Schiemenz, Sandra; Goennenwein, Sebastian T.B.; Nielsch, Kornelius; Leistner, Karin
    The perspective of energy-efficient and tunable functional magnetic nanostructures has triggered research efforts in the fields of voltage control of magnetism and spintronics. We investigate the magnetotransport properties of nanocomposite iron oxide/iron thin films with a nominal iron thickness of 5-50 nm and find a positive magnetoresistance at small thicknesses. The highest magnetoresistance was found for 30 nm Fe with +1.1% at 3 T. This anomalous behavior is attributed to the presence of Fe3O4-Fe nanocomposite regions due to grain boundary oxidation. At the Fe3O4/Fe interfaces, spin-polarized electrons in the magnetite can be scattered and reoriented. A crossover to negative magnetoresistance (-0.11%) is achieved at a larger thickness (>40 nm) when interface scattering effects become negligible as more current flows through the iron layer. Electrolytic gating of this system induces voltage-triggered redox reactions in the Fe3O4 regions and thereby enables voltage-tuning of the magnetoresistance with the locally oxidized regions as the active tuning elements. In the low-magnetic-field region (<1 T), a crossover from positive to negative magnetoresistance is achieved by a voltage change of only 1.72 V. At 3 T, a relative change of magnetoresistance about -45% during reduction was achieved for the 30 nm Fe sample. The present low-voltage approach signifies a step forward to practical and tunable room-temperature magnetoresistance-based nanodevices, which can boost the development of nanoscale and energy-efficient magnetic field sensors with high sensitivity, magnetic memories, and magnetoelectric devices in general. Copyright © 2020 American Chemical Society.
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    Structural and Electric Properties of Epitaxial Na0.5Bi0.5TiO3-Based Thin Films
    (Basel : MDPI, 2021) Magalhaes, Bruno; Engelhardt, Stefan; Molin, Christian; Gebhardt, Sylvia E.; Nielsch, Kornelius; Hühne, Ruben
    Substantial efforts are dedicated worldwide to use lead-free materials for environmentally friendly processes in electrocaloric cooling. Whereas investigations on bulk materials showed that Na0.5Bi0.5TiO3 (NBT)-based compounds might be suitable for such applications, our aim is to clarify the feasibility of epitaxial NBT-based thin films for more detailed investigations on the correlation between the composition, microstructure, and functional properties. Therefore, NBT-based thin films were grown by pulsed laser deposition on different single crystalline substrates using a thin epitaxial La0.5Sr0.5CoO3 layer as the bottom electrode for subsequent electric measurements. Structural characterization revealed an undisturbed epitaxial growth of NBT on lattice-matching substrates with a columnar microstructure, but high roughness and increasing grain size with larger film thickness. Dielectric measurements indicate a shift of the phase transition to lower temperatures compared to bulk samples as well as a reduced permittivity and increased losses at higher temperatures. Whereas polarization loops taken at −100 °C revealed a distinct ferroelectric behavior, room temperature data showed a significant resistive contribution in these measurements. Leakage current studies confirmed a non-negligible conductivity between the electrodes, thus preventing an indirect characterization of the electrocaloric properties of these films.
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    Influence of Nanoparticle Processing on the Thermoelectric Properties of (BixSb1−X)2Te3 Ternary Alloys
    (Weinheim : Wiley-VCH, 2021) Salloum, Sarah; Bendt, Georg; Heidelmann, Markus; Loza, Kateryna; Bayesteh, Samaneh; Izadi, M. Sepideh; Patrick, Kawulok; He, Ran; Schlörb, Heike; Perez, Nicolas; Reith, Heiko; Nielsch, Kornelius; Schierning, Gabi; Schulz, Stephan
    The synthesis of phase‐pure ternary solutions of tetradymite‐type materials (BixSb1−x)2Te3 (x=0.25; 0.50; 0.75) in an ionic liquid approach has been carried out. The nanoparticles are characterized by means of energy‐dispersive X‐ray spectroscopy (EDX), powder X‐ray diffraction (PXRD), scanning electron microscopy (SEM), and transmission electron microscopy. In addition, the role of different processing approaches on the thermoelectric properties ‐ Seebeck coefficient as well as electrical and thermal conductivity ‐ is demonstrated.