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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
- 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.
- ItemHow to grow single-crystalline and epitaxial NiTi films in (100)- and (111)-orientation(Bristol : IOP Publishing, 2023) Lünser, Klara; Undisz, Andreas; Nielsch, Kornelius; Fähler, SebastianUnderstanding the martensitic microstructure in nickel-titanium (NiTi) thin films helps to optimize their properties for applications in microsystems. Epitaxial and single-crystalline films can serve as model systems to understand the microstructure, as well as to exploit the anisotropic mechanical properties of NiTi. Here, we analyze the growth of NiTi on single-crystalline MgO(100) and Al2O3(0001) substrates and optimize film and buffer deposition conditions to achieve epitaxial films in (100)- and (111)-orientation. On MgO(100), we compare the transformation behavior and crystal quality of (100)-oriented NiTi films on different buffer layers. We demonstrate that a vanadium buffer layer helps to decrease the low-angle grain boundary density in the NiTi film, which inhibits undesired growth twins and leads to higher transformation temperatures. On Al2O3(0001), we analyze the orientation of a chromium buffer layer and find that it grows (111)-oriented only in a narrow temperature range around 500 ∘C. By depositing the Cr buffer below the NiTi film, we can prepare (111)-oriented, epitaxial films with transformation temperatures above room temperature. Transmission electron microscopy confirms a martensitic microstructure with Guinier Preston-zone precipitates at room temperature. We identify the deposition conditions to approach the ideal single crystalline state, which is beneficial for the analysis of the martensitic microstructure and anisotropic mechanical properties in different film orientations.
- 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.
- 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
- ItemElectrochemical nanostructuring of (111) oriented GaAs crystals: From porous structures to nanowires(Frankfurt, M. : Beilstein-Institut zur Förderung der Chemischen Wissenschaften, 2020) Monaico, Elena I.; Monaico, Eduard V.; Ursaki, Veaceslav V.; Honnali, Shashank; Postolache, Vitalie; Leistner, Karin; Nielsch, Kornelius; Tiginyanu, Ion M.A comparative study of the anodization processes occurring at the GaAs(111)A and GaAs(111)B surfaces exposed to electrochemical etching in neutral NaCl and acidic HNO3 aqueous electrolytes is performed in galvanostatic and potentiostatic anodization modes. Anodization in NaCl electrolytes was found to result in the formation of porous structures with porosity controlled either by current under the galvanostatic anodization, or by the potential under the potentiostatic anodization. Possibilities to produce multilayer porous structures are demonstrated. At the same time, one-step anodization in a HNO3 electrolyte is shown to lead to the formation of GaAs triangular shape nanowires with high aspect ratio (400 nm in diameter and 100 μm in length). The new data are compared to those previously obtained through anodizing GaAs(100) wafers in alkaline KOH electrolyte. An IR photodetector based on the GaAs nanowires is demonstrated. © 2020 Monaico et al.
- ItemInfluence of Alumina Addition on the Optical Properties and the Thermal Stability of Titania Thin Films and Inverse Opals Produced by Atomic Layer Deposition(Basel : MDPI, 2021) Waleczek, Martin; Dendooven, Jolien; Dyachenko, Pavel; Petrov, Alexander Y.; Eich, Manfred; Blick, Robert H.; Detavernier, Christophe; Nielsch, Kornelius; Furian, Kaline P.; Zierold, RobertTiO2 thin films deposited by atomic layer deposition (ALD) at low temperatures (<100 °C) are, in general, amorphous and exhibit a smaller refractive index in comparison to their crystalline counterparts. Nonetheless, low-temperature ALD is needed when the substrates or templates are based on polymeric materials, as the deposition has to be performed below their glass transition or melting temperatures. This is the case for photonic crystals generated via ALD infiltration of self-assembled polystyrene templates. When heated up, crystal phase transformations take place in the thin films or photonic structures, and the accompanying volume reduction as well as the burn-out of residual impurities can lead to mechanical instability. The introduction of cation doping (e.g., Al or Nb) in bulk TiO2 parts is known to alter phase transitions and to stabilize crystalline phases. In this work, we have developed low-temperature ALD super-cycles to introduce Al2O3 into TiO2 thin films and photonic crystals. The aluminum oxide content was adjusted by varying the TiO2:Al2O3 internal loop ratio within the ALD super-cycle. Both thin films and inverse opal photonic crystal structures were subjected to thermal treatments ranging from 200 to 1200 °C and were characterized by in- and ex-situ X-ray diffraction, spectroscopic ellipsometry, and spectroscopic reflectance measurements. The results show that the introduction of alumina affects the crystallization and phase transition temperatures of titania as well as the optical properties of the inverse opal photonic crystals (iPhC). The thermal stability of the titania iPhCs was increased by the alumina introduction, maintaining their photonic bandgap even after heat treatment at 900 °C and outperforming the pure titania, with the best results being achieved with the super-cycles corresponding to an estimated alumina content of 26 wt.%.
- ItemSignatures of a Charge Density Wave Phase and the Chiral Anomaly in the Fermionic Material Cobalt Monosilicide CoSi(Weinheim : Wiley-VCH Verlag GmbH & Co. KG, 2020) Schnatmann, Lauritz; Geishendorf, Kevin; Lammel, Michaela; Damm, Christine; Novikov, Sergey; Thomas, Andy; Burkov, Alexander; Reith, Heiko; Nielsch, Kornelius; Schierning, GabiMaterials with topological electronic states have emerged as one of the most exciting discoveries of condensed quantum matter, hosting quasiparticles with extremely low effective mass and high mobility. Weyl materials contain such topological states in the bulk and additionally have a non-trivial chiral charge. However, despite known quantum effects caused by these chiral states, the interplay between chiral states, and a charge density wave phase, an ordering of the electrons to a correlated phase is not experimentally explored. Indications for the formation of a charge density wave phase in the Weyl material cobalt monosilicide CoSi are observed. Furthermore, the typical signatures of the charge density wave phase together with typical signatures of Weyl fermions in magnetic field dependent electrical transport characterization are investigated. The charge density wave and the chiral contribution to the electrical magneto-transport are separated as well as a suppression of the charge density wave phase is observed in magnetic fields. © 2019 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
- ItemWater-Free SbOx ALD Process for Coating Bi2Te3 Particle(Basel : MDPI, 2023) Lehmann, Sebastian; Mitzscherling, Fanny; He, Shiyang; Yang, Jun; Hantusch, Martin; Nielsch, Kornelius; Bahrami, AminWe developed a water-free atomic layer deposition (ALD) process to homogeneously deposit SbOx using SbCl5 and Sb-Ethoxide as precursors, and report it here for the first time. The coating is applied on Bi2Te3 particles synthesized via the solvothermal route to enhance the thermoelectric properties (i.e., Seebeck coefficient, thermal and electrical conductivity) via interface engineering. The amorphous character of the coating was shown by the missing reflexes on the X-ray diffractograms (XRD). A shift from the oxidation state +III to +V of the Sb species was observed using X-ray photoelectron spectroscopy (XPS), indicating increased thickness of the SbOx coating layer. Additionally, a peak shift of the Sb 3d5/2 + O 1s peak indicated increased n-type doping of the material. Electrical measurements of spark plasma-sintered bulk samples confirmed the doping effect on the basis of decreased specific resistivity with increasing SbOx layer thickness. The Seebeck coefficient was improved for the coated sample with 500 cycles of SbOx, while the total thermal conductivity was reduced, resulting in enhancement of the zT. The results distinctly show that surface engineering via powder ALD is an effective tool for improving key properties of thermoelectric materials like electrical conductivity and the Seebeck coefficient.
- ItemStructural 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, RubenSubstantial 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.