Browsing by Author "Schierning, Gabi"
Now showing 1 - 14 of 14
Results Per Page
- ItemDensity-Dependence of Surface Transport in Tellurium-Enriched Nanograined Bulk Bi2Te3(Weinheim : Wiley-VCH, 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, GabiThree-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.
- ItemDoping High-Mobility Donor : Acceptor Copolymer Semiconductors with an Organic Salt for High-Performance Thermoelectric Materials(Weinheim : Wiley-VCH Verlag GmbH & Co. KG, 2020) Guo, Jing; Li, Guodong; Reith, Heiko; Jiang, Lang; Wang, Ming; Li, Yuhao; Wang, Xinhao; Zeng, Zebing; Zhao, Huaizhou; Lu, Xinhui; Schierning, Gabi; Nielsch, Kornelius; Liao, Lei; Hu, YuanyuanOrganic semiconductors (OSCs) are attractive for fabrication of thermoelectric devices with low cost, large area, low toxicity, and high flexibility. In order to achieve high-performance organic thermoelectric devices (OTEs), it is essential to develop OSCs with high conductivity (σ), large Seebeck coefficient (S), and low thermal conductivity (κ). It is equally important to explore efficient dopants matching the need of thermoelectric devices. The thermoelectric performance of a high-mobility donor–acceptor (D–A) polymer semiconductor, which is doped by an organic salt, is studied. Both a high p-type electrical conductivity approaching 4 S cm−1 and an excellent power factor (PF) of 7 µW K−2 m−1 are obtained, which are among the highest reported values for polymer semiconductors. Temperature-dependent conductivity, Seebeck coefficient and power factor of the doped materials are systematically investigated. Detailed analysis on the results of thermoelectric measurements has revealed a hopping transport in the materials, which verifies the empirical relationship: S ∝ σ−1/4 and PF ∝ σ1/2. The results demonstrate that D–A copolymer semiconductors with proper combination of dopants have great potential for fabricating high-performance thermoelectric devices. © 2020 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
- ItemEuropium Clustering and Glassy Magnetic Behavior in Inorganic Clathrate-VIII Eu8Ga16Ge30(Basel : MDPI, 2022) Pérez, Nicolás; Sahoo, Manaswini; Schierning, Gabi; Nielsch, Kornelius; Nolas, George S.The temperature- and field-dependent, electrical and thermal properties of inorganic clathrate-VIII Eu8Ga16Ge30 were investigated. The type VIII clathrates were obtained from the melt of elements as reported previously. Specifically, the electrical resistivity data show hysteretic magnetoresistance at low temperatures, and the Seebeck coefficient and Hall data indicate magnetic interactions that affect the electronic structure in this material. Heat capacity and thermal conductivity data corroborate these findings and reveal the complex behavior due to Eu2+ magnetic ordering and clustering from approximately 13 to 4 K. Moreover, the low-frequency dynamic response indicates Eu8Ga16Ge30 to be a glassy magnetic system. In addition to advancing our fundamental understanding of the physical properties of this material, our results can be used to further the research for potential applications of interest in the fields of magnetocalorics or thermoelectrics.
- ItemHeterostructured Bismuth Telluride Selenide Nanosheets for Enhanced Thermoelectric Performance(Weinheim : Wiley-VCH GmbH, 2020) Bauer, Christoph; Veremchuk, Igor; Kunze, Christof; Benad, Albrecht; Dzhagan, Volodymyr M.; Haubold, Danny; Pohl, Darius; Schierning, Gabi; Nielsch, Kornelius; Lesnyak, Vladimir; Eychmüller, AlexanderThe n-type semiconductor system Bi2Te3Bi2Se3 is known as a low-temperature thermoelectric material with a potentially high efficiency. Herein, a facile approach is reported to synthesize core/shell heterostructured Bi2Te2Se/Bi2Te3 nanosheets (NSs) with lateral dimensions of 1-3 mu m and thickness of about 50nm. Bi2Te3 and Bi2Se3, as well as heterostructured Bi2Te2Se/Bi2Te3 NSs are obtained via colloidal synthesis. Heterostructured NSs show an inhomogeneous distribution of the chalcogen atoms forming selenium and tellurium-rich layers across the NS thickness, resulting in a core/shell structure. Detailed morphological studies reveal that these structures contain nanosized pores. These features contribute to the overall thermoelectric properties of the material, inducing strong phonon scattering at grain boundaries in compacted solids. NSs are processed into nanostructured bulks through spark plasma sintering of dry powders to form a thermoelectric material with high power factor. Electrical characterization of our materials reveals a strong anisotropic behavior in consolidated pellets. It is further demonstrated that by simple thermal annealing, core/shell structure can be controllably transformed into alloyed one. Using this approach pellets with Bi2Te2.55Se0.45 composition are obtained, which exhibit low thermal conductivity and high power factor for in-plane direction with zT of 1.34 at 400K.
- ItemImproving the zT value of thermoelectrics by nanostructuring: Tuning the nanoparticle morphology of Sb2Te3 by using ionic liquids(Cambridge : Royal Society of Chemistry, 2016) Schaumann, Julian; Loor, Manuel; Ünal, Derya; Mudring, Anja; Heimann, Stefan; Hagemann, Ulrich; Schulz, Stephan; Maculewicz, Franziska; Schierning, GabiA systematic study on the microwave-assisted thermolysis of the single source precursor (Et2Sb)2Te (1) in different asymmetric 1-alkyl-3-methylimidazolium- and symmetric 1,3-dialkylimidazolium-based ionic liquids (ILs) reveals the distinctive role of both the anion and the cation in tuning the morphology and microstructure of the resulting Sb2Te3 nanoparticles as evidenced by X-ray diffraction (XRD), scanning electron microscopy (SEM), energy dispersive X-ray analysis (EDX), and X-ray photoelectron spectroscopy (XPS). A comparison of the electrical and thermal conductivities as well as the Seebeck coefficient of the Sb2Te3 nanoparticles obtained from different ILs reveals the strong influence of the specific IL, from which C4mimI was identified as the best solvent, on the thermoelectric properties of as-prepared nanosized Sb2Te3. This work provides design guidelines for ILs, which allow the synthesis of nanostructured thermoelectrics with improved performances.
- 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.
- ItemPolyethenetetrathiolate or polytetrathiooxalate? Improved synthesis, a comparative analysis of a prominent thermoelectric polymer and implications to the charge transport mechanism(Cambridge : RSC Publ., 2018) Tkachov, Roman; Stepien, Lukas; Grafe, Robert; Guskova, Olga; Kiriy, Anton; Simon, Frank; Reith, Heiko; Nielsch, Kornelius; Schierning, Gabi; Kasinathan, Deepa; Leyens, Christoph1,1,2,2-Ethenetetrathiolate (ett4-) coordination polymers, such as poly[Kx(Ni-ett)], have been known for decades for their excellent thermoelectric properties. However in reality, ett4- is neither a "true" comonomer which participates in the polymerization, nor represents a "true" repeat unit of the target polymer. Indeed, poly[K2(Ni-ett)], which is formally the product of Ni-induced polymerization of ett4-, has a poor conductivity and needs to be oxidized to show attractive thermoelectric characteristics. The polymerization and oxidation processes are poorly controllable which causes irreproducibility of the polymer properties. To improve the synthesis reproducibility, we studied polymerization of potassium tetrathiooxalate (K2tto), the convenient synthesis of which was developed in our recent work. Because K2tto is the "true monomer", and not its precursor, a high quality product is reproducibly formed simply by mixing K2tto with NiCl2 at room temperature. The procedure does not require additional components (bases), or special conditions (prolonged heating), which are usually needed for the preparation of this polymer from the monomer precursor 1,3,4,6-tetrathiapentalene-2,5-dione (TPD). Furthermore, as tto2- is formally the product of two-electron oxidation of ett4-, the poorly controllable oxidation process is avoided and poly[Ni-tto] almost free from K is directly formed upon the complexation of Ni2+ and tto2-. Thus-obtained poly[Ni-tto] possesses conductivity in the range of 27-47 S cm-1 and a Seebeck coefficient in the range of -38 to -55 μV K-1, which are superior thermoelectric properties compared to poly[Kx(Ni-ett)] samples obtained by the previously reported methods. Redox and structural properties of poly[Ni-tto] were compared with those of poly[Kx(Ni-ett)] obtained by the reported methods. Furthermore, DFT calculations were performed to shed more light on generally promising properties of this class of materials. Particularly, possible packing models have been predicted for polymers, and the molecular dynamics simulations have been used to simulate the molecular arrangements under ambient conditions.
- 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.
- ItemThermoelectric 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, HeikoSuccessful 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
- ItemTowards tellurium-free thermoelectric modules for power generation from low-grade heat(London : Nature Publishing Group, 2021) Ying, Pingjun; He, Ran; Mao, Jun; Zhang, Qihao; Reith, Heiko; Sui, Jiehe; Ren, Zhifeng; Nielsch, Kornelius; Schierning, GabiThermoelectric technology converts heat into electricity directly and is a promising source of clean electricity. Commercial thermoelectric modules have relied on Bi2Te3-based compounds because of their unparalleled thermoelectric properties at temperatures associated with low-grade heat (<550 K). However, the scarcity of elemental Te greatly limits the applicability of such modules. Here we report the performance of thermoelectric modules assembled from Bi2Te3-substitute compounds, including p-type MgAgSb and n-type Mg3(Sb,Bi)2, by using a simple, versatile, and thus scalable processing routine. For a temperature difference of ~250 K, whereas a single-stage module displayed a conversion efficiency of ~6.5%, a module using segmented n-type legs displayed a record efficiency of ~7.0% that is comparable to the state-of-the-art Bi2Te3-based thermoelectric modules. Our work demonstrates the feasibility and scalability of high-performance thermoelectric modules based on sustainable elements for recovering low-grade heat.
- 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.
- ItemUnveiling the phonon scattering mechanisms in half-Heusler thermoelectric compounds(Cambridge : RSC Publ., 2020) He, Ran; Zhu, Taishan; Wang, Yumei; Wolff, Ulrike; Jaud, Jean-Christophe; Sotnikov, Andrei; Potapov, Pavel; Wolf, Daniel; Ying, Pingjun; Wood, Max; Liu, Zhenhui; Feng, Le; Perez Rodriguez, Nicolas; Snyder, G. Jeffrey; Grossman, Jeffrey C.; Nielsch, Kornelius; Schierning, GabiHalf-Heusler (HH) compounds are among the most promising thermoelectric (TE) materials for large-scale applications due to their superior properties such as high power factor, excellent mechanical and thermal reliability, and non-toxicity. Their only drawback is the remaining-high lattice thermal conductivity. Various mechanisms were reported with claimed effectiveness to enhance the phonon scattering of HH compounds including grain-boundary scattering, phase separation, and electron–phonon interaction. In this work, however, we show that point-defect scattering has been the dominant mechanism for phonon scattering other than the intrinsic phonon–phonon interaction for ZrCoSb and possibly many other HH compounds. Induced by the charge-compensation effect, the formation of Co/4d Frenkel point defects is responsible for the drastic reduction of lattice thermal conductivity in ZrCoSb1−xSnx. Our work systematically depicts the phonon scattering profile of HH compounds and illuminates subsequent material optimizations.
- 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.