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Rare-earth-free MnAl-C-Ni permanent magnets produced by extrusion of powder milled from bulk

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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The Role of Al2O3 ALD Coating on Sn-Based Intermetallic Anodes for Rate Capability and Long-Term Cycling in Lithium-Ion Batteries

2022, Soltani, Niloofar, Abbas, Syed Muhammad, Hantusch, Martin, Lehmann, Sebastian, Nielsch, Kornelius, Bahrami, Amin, Mikhailova, Daria

The electrochemical performances of CoSn2 and Ni3Sn4 as potential anode materials in lithium-ion batteries (LIBs) are investigated using varying thicknesses of an alumina layer deposited by the atomic layer deposition (ALD) technique. Rate capability results showed that at high current densities, Al2O3-coated CoSn2 and Ni3Sn4 electrodes after 10-ALD cycles outperformed uncoated materials. The charge capacities of coated CoSn2 and Ni3Sn4 electrodes are 571 and 134 mAh g−1, respectively, at a high current density of 5 A g−1, while the capacities of uncoated electrodes are 363 and 11 mAh g−1. When the current density is reduced to 1 A g−1, however, the cycling performances of Al2O3-coated CoSn2 and Ni3Sn4 electrodes fade faster after almost 40 cycles than uncoated electrodes. The explanation is found in the composition of the solid-electrolyte interface (SEI), which strongly depends on the current rate. Thus, X-ray photoelectron spectroscopy analysis of SEI layers on coated samples cycles at a low current density of 0.1 Ag−1, revealed organic carbonates as major products, which probably have a low ionic conductivity. In contrast, the SEI of coated materials cycled at 5 Ag−1 consists mostly of mixed inorganic/organic fluorine-rich Al-F and C-F species facilitating a higher ionic transport, which improves electrochemical performance.

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Thermoelectric Characterization Platform for Electrochemically Deposited Materials

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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Current State-of-the-Art in the Interface/Surface Modification of Thermoelectric Materials

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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On Curie temperature of B20-MnSi films

2022, Li, Zichao, Yuan, Ye, Begeza, Viktor, Rebohle, Lars, Helm, Manfred, Nielsch, Kornelius, Prucnal, Slawomir, Zhou, Shengqiang

B20-type MnSi is the prototype magnetic skyrmion material. Thin films of MnSi show a higher Curie temperature than their bulk counterpart. However, it is not yet clear what mechanism leads to the increase of the Curie temperature. In this work, we grow MnSi films on Si(100) and Si(111) substrates with a broad variation in their structures. By controlling the Mn thickness and annealing parameters, the pure MnSi phase of polycrystalline and textured nature as well as the mixed phase of MnSi and MnSi1.7 are obtained. Surprisingly, all these MnSi films show an increased Curie temperature of up to around 43 K. The Curie temperature is likely independent of the structural parameters within our accessibility including the film thickness above a threshold, strain, cell volume and the mixture with MnSi1.7. However, a pronounced phonon softening is observed for all samples, which can tentatively be attributed to slight Mn excess from stoichiometry, leading to the increased Curie temperature.

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Self‐Patterning of Multifunctional Heusler Membranes by Dewetting

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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Transparent Power-Generating Windows Based on Solar-Thermal-Electric Conversion

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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Density-Dependence of Surface Transport in Tellurium-Enriched Nanograined Bulk Bi2Te3

2023, Izadi, Sepideh, Bhattacharya, Ahana, Salloum, Sarah, Han, Jeong Woo, Schnatmann, Lauritz, Wolff, Ulrike, Perez, Nicolas, Bendt, Georg, Ennen, Inga, Hütten, Andreas, Nielsch, Kornelius, Schulz, Stephan, Mittendorff, Martin, Schierning, Gabi

Three-dimensional topological insulators (3D TI) exhibit conventional parabolic bulk bands and protected Dirac surface states. A thorough investigation of the different transport channels provided by the bulk and surface carriers using macroscopic samples may provide a path toward accessing superior surface transport properties. Bi2Te3 materials make promising 3D TI models; however, due to their complicated defect chemistry, these materials have a high number of charge carriers in the bulk that dominate the transport, even as nanograined structures. To partially control the bulk charge carrier density, herein the synthesis of Te-enriched Bi2Te3 nanoparticles is reported. The resulting nanoparticles are compacted into nanograined pellets of varying porosity to tailor the surface-to-volume ratio, thereby emphasizing the surface transport channels. The nanograined pellets are characterized by a combination of resistivity, Hall- and magneto-conductance measurements together with (THz) time-domain reflectivity measurements. Using the Hikami-Larkin-Nagaoka (HLN) model, a characteristic coherence length of ≈200 nm is reported that is considerably larger than the diameter of the nanograins. The different contributions from the bulk and surface carriers are disentangled by THz spectroscopy, thus emphasizing the dominant role of the surface carriers. The results strongly suggest that the surface transport carriers have overcome the hindrance imposed by nanoparticle boundaries.

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Building Hierarchical Martensite

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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Voltage‐Controlled Deblocking of Magnetization Reversal in Thin Films by Tunable Domain Wall Interactions and Pinning Sites

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.