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- ItemSelf‐Patterning of Multifunctional Heusler Membranes by Dewetting(Weinheim : Wiley-VCH, 2021) Lünser, Klara; Diestel, Anett; Nielsch, Kornelius; Fähler, SebastianNi-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
- ItemBuilding 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, SebastianMartensitic 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
- ItemTransparent 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, LidongIntegrating 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.
- ItemCurrent State-of-the-Art in the Interface/Surface Modification of Thermoelectric Materials(Weinheim : Wiley-VCH, 2021) He, Shiyang; Lehmann, Sebastian; Bahrami, Amin; Nielsch, KorneliusThermoelectric (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.
- ItemInfluence 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, StephanThe 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.
- ItemInterface-Dominated Topological Transport in Nanograined Bulk Bi2 Te3(Weinheim : Wiley-VCH, 2021) Izadi, Sepideh; Han, Jeong Woo; Salloum, Sarah; Wolff, Ulrike; Schnatmann, Lauritz; Asaithambi, Aswin; Matschy, Sebastian; Schlörb, Heike; Reith, Heiko; Perez, Nicolas; Nielsch, Kornelius; Schulz, Stephan; Mittendorff, Martin; Schierning, Gabi3D topological insulators (TI) host surface carriers with extremely high mobility. However, their transport properties are typically dominated by bulk carriers that outnumber the surface carriers by orders of magnitude. A strategy is herein presented to overcome the problem of bulk carrier domination by using 3D TI nanoparticles, which are compacted by hot pressing to macroscopic nanograined bulk samples. Bi2Te3 nanoparticles well known for their excellent thermoelectric and 3D TI properties serve as the model system. As key enabler for this approach, a specific synthesis is applied that creates nanoparticles with a low level of impurities and surface contamination. The compacted nanograined bulk contains a high number of interfaces and grain boundaries. Here it is shown that these samples exhibit metallic-like electrical transport properties and a distinct weak antilocalization. A downward trend in the electrical resistivity at temperatures below 5 K is attributed to an increase in the coherence length by applying the Hikami–Larkin–Nagaoka model. THz time-domain spectroscopy reveals a dominance of the surface transport at low frequencies with a mobility of above 103 cm2 V−1 s−1 even at room temperature. These findings clearly demonstrate that nanograined bulk Bi2Te3 features surface carrier properties that are of importance for technical applications.
- ItemHigh-Pressure-Sintering-Induced Microstructural Engineering for an Ultimate Phonon Scattering of Thermoelectric Half-Heusler Compounds(Weinheim : Wiley-VCH, 2021) He, Ran; Zhu, Taishan; Ying, Pingjun; Chen, Jie; Giebeler, Lars; Kühn, Uta; Grossman, Jeffrey C.; Wang, Yumei; Nielsch, KorneliusThermal management is of vital importance in various modern technologies such as portable electronics, photovoltaics, and thermoelectric devices. Impeding phonon transport remains one of the most challenging tasks for improving the thermoelectric performance of certain materials such as half-Heusler compounds. Herein, a significant reduction of lattice thermal conductivity (κL) is achieved by applying a pressure of ≈1 GPa to sinter a broad range of half-Heusler compounds. Contrasting with the common sintering pressure of less than 100 MPa, the gigapascal-level pressure enables densification at a lower temperature, thus greatly modifying the structural characteristics for an intensified phonon scattering. A maximum κL reduction of ≈83% is realized for HfCoSb from 14 to 2.5 W m−1 K−1 at 300 K with more than 95% relative density. The realized low κL originates from a remarkable grain-size refinement to below 100 nm together with the abundant in-grain defects, as determined by microscopy investigations. This work uncovers the phonon transport properties of half-Heusler compounds under unconventional microstructures, thus showing the potential of high-pressure compaction in advancing the performance of thermoelectric materials.
- ItemIncreasing the Diversity and Understanding of Semiconductor Nanoplatelets by Colloidal Atomic Layer Deposition(Weinheim : Wiley-VCH, 2020) Reichhelm, Annett; Hübner, René; Damm, Christine; Nielsch, Kornelius; Eychmüller, AlexanderNanoplatelets (NPLs) are a remarkable class of quantum confined materials with size-dependent optical properties, which are determined by the defined thickness of the crystalline platelets. To increase the variety of species, the colloidal atomic layer deposition method is used for the preparation of increasingly thicker CdSe NPLs. By growing further crystalline layers onto the surfaces of 4 and 5 monolayers (MLs) thick NPLs, species from 6 to 13 MLs are achieved. While increasing the thickness, the heavy-hole absorption peak shifts from 513 to 652 nm, leading to a variety of NPLs for applications and further investigations. The thickness and number of MLs of the platelet species are determined by high-resolution transmission electron microscopy (HRTEM) measurements, allowing the interpretation of several contradictions present in the NPL literature. In recent years, different assumptions are published, leading to a lack of clarity in the fundamentals of this field. Regarding the ongoing scientific interest in NPLs, there is a certain need for clarification, which is provided in this study. © 2020 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
- ItemPhase Selection in Mn–Si Alloys by Fast Solid-State Reaction with Enhanced Skyrmion Stability(Weinheim : Wiley-VCH, 2021) Li, Zichao; Xie, Yufang; Yuan, Ye; Ji, Yanda; Begeza, Viktor; Cao, Lei; Hübner, René; Rebohle, Lars; Helm, Manfred; Nielsch, Kornelius; Prucnal, Slawomir; Zhou, ShengqiangB20-type transition-metal silicides or germanides are noncentrosymmetric materials hosting magnetic skyrmions, which are promising information carriers in spintronic devices. The prerequisite is to prepare thin films on technology-relevant substrates with magnetic skyrmions stabilized at a broad temperature and magnetic-field working window. A canonical example is the B20-MnSi film grown on Si substrates. However, the as-yet unavoidable contamination with MnSi1.7 occurs due to the lower nucleation temperature of this phase. In this work, a simple and efficient method to overcome this problem and prepare single-phase MnSi films on Si substrates is reported. It is based on the millisecond reaction between metallic Mn and Si using flash-lamp annealing (FLA). By controlling the FLA energy density, single-phase MnSi or MnSi1.7 or their mixture can be grown at will. Compared with bulk MnSi, the prepared MnSi films show an increased Curie temperature of up to 41 K. In particular, the magnetic skyrmions are stable over a much wider temperature and magnetic-field range than reported previously. The results constitute a novel phase selection approach for alloys and can help to enhance specific functional properties, such as the stability of magnetic skyrmions. © 2021 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH
- ItemWaste Recycling in Thermoelectric Materials(Weinheim : Wiley-VCH, 2020) Bahrami, Amin; Schierning, Gabi; Nielsch, KorneliusThermoelectric (TE) technology enables the efficient conversion of waste heat generated in homes, transport, and industry into promptly accessible electrical energy. Such technology is thus finding increasing applications given the focus on alternative sources of energy. However, the synthesis of TE materials relies on costly and scarce elements, which are also environmentally damaging to extract. Moreover, spent TE modules lead to a waste of resources and cause severe pollution. To address these issues, many laboratory studies have explored the synthesis of TE materials using wastes and the recovery of scarce elements from spent modules, e.g., utilization of Si slurry as starting materials, development of biodegradable TE papers, and bacterial recovery and recycling of tellurium from spent TE modules. Yet, the outcomes of such work have not triggered sustainable industrial practices to the extent needed. This paper provides a systematic overview of the state of the art with a view to uncovering the opportunities and challenges for expanded application. Based on this overview, it explores a framework for synthesizing TE materials from waste sources with efficiencies comparable to those made from raw materials.