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- ItemA Holistic Solution to Icing by Acoustic Waves: De-Icing, Active Anti-Icing, Sensing with Piezoelectric Crystals, and Synergy with Thin Film Passive Anti-Icing Solutions(Weinheim : Wiley-VCH, 2023) del Moral, Jaime; Montes, Laura; Rico‐Gavira, Victor Joaquin; López‐Santos, Carmen; Jacob, Stefan; Oliva‐Ramirez, Manuel; Gil‐Rostra, Jorge; Fakhfouri, Armaghan; Pandey, Shilpi; Gonzalez del Val, Miguel; Mora, Julio; García‐Gallego, Paloma; Ibáñez‐Ibáñez, Pablo Francisco; Rodríguez‐Valverde, Miguel Angel; Winkler, Andreas; Borrás, Ana; González‐Elipe, Agustin RodriguezIcing has become a hot topic both in academia and in the industry given its implications in transport, wind turbines, photovoltaics, and telecommunications. Recently proposed de-icing solutions involving the propagation of acoustic waves (AWs) at suitable substrates may open the path for a sustainable alternative to standard de-icing or anti-icing procedures. Herein, the fundamental interactions are unraveled that contribute to the de-icing and/or hinder the icing on AW-activated substrates. The response toward icing of a reliable model system consisting of a piezoelectric plate activated by extended electrodes is characterized at a laboratory scale and in an icing wind tunnel under realistic conditions. Experiments show that surface modification with anti-icing functionalities provides a synergistic response when activated with AWs. A thoughtful analysis of the resonance frequency dependence on experimental variables such as temperature, ice formation, or wind velocity demonstrates the application of AW devices for real-time monitoring of icing processes.
- ItemCharge‐Compensated N‐Doped π ‐Conjugated Polymers: Toward both Thermodynamic Stability of N‐Doped States in Water and High Electron Conductivity(Weinheim : Wiley-VCH, 2022) Borrmann, Fabian; Tsuda, Takuya; Guskova, Olga; Kiriy, Nataliya; Hoffmann, Cedric; Neusser, David; Ludwigs, Sabine; Lappan, Uwe; Simon, Frank; Geisler, Martin; Debnath, Bipasha; Krupskaya, Yulia; Al‐Hussein, Mahmoud; Kiriy, AntonThe understanding and applications of electron-conducting π-conjugated polymers with naphtalene diimide (NDI) blocks show remarkable progress in recent years. Such polymers demonstrate a facilitated n-doping due to the strong electron deficiency of the main polymer chain and the presence of the positively charged side groups stabilizing a negative charge of the n-doped backbone. Here, the n-type conducting NDI polymer with enhanced stability of its n-doped states for prospective “in-water” applications is developed. A combined experimental–theoretical approach is used to identify critical features and parameters that control the doping and electron transport process. The facilitated polymer reduction ability and the thermodynamic stability in water are confirmed by electrochemical measurements and doping studies. This material also demonstrates a high conductivity of 10−2 S cm−1 under ambient conditions and 10−1 S cm−1 in vacuum. The modeling explains the stabilizing effects for various dopants. The simulations show a significant doping-induced “collapse” of the positively charged side chains on the core bearing a partial negative charge. This explains a decrease in the lamellar spacing observed in experiments. This study fundamentally enables a novel pathway for achieving both thermodynamic stability of the n-doped states in water and the high electron conductivity of polymers.
- 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
- ItemPhotoluminescence Mapping over Laser Pulse Fluence and Repetition Rate as a Fingerprint of Charge and Defect Dynamics in Perovskites(Weinheim : Wiley-VCH, 2023) Rao, Shraddha M.; Kiligaridis, Alexander; Yangui, Aymen; An, Qingzhi; Vaynzof, Yana; Scheblykin, Ivan G.Defects in metal halide perovskites (MHP) are photosensitive, making the observer effect unavoidable when laser spectroscopy methods are applied. Photoluminescence (PL) bleaching and enhancement under light soaking and recovery in dark are examples of the transient phenomena that are consequent to the creation and healing of defects. Depending on the initial sample composition, environment, and other factors, the defect nature and evolution can strongly vary, making spectroscopic data analysis prone to misinterpretations. Herein, the use of an automatically acquired dependence of PL quantum yield (PLQY) on the laser pulse repetition rate and pulse fluence as a unique fingerprint of both charge carrier dynamics and defect evolution is demonstrated. A simple visual comparison of such fingerprints allows for assessment of similarities and differences between MHP samples. The study illustrates this by examining methylammonium lead triiodide (MAPbI3) films with altered stoichiometry that just after preparation showed very pronounced defect dynamics at time scale from milliseconds to seconds, clearly distorting the PLQY fingerprint. Upon weeks of storage, the sample fingerprints evolve toward the standard stoichiometric MAPbI3 in terms of both charge carrier dynamics and defect stability. Automatic PLQY mapping can be used as a universal method for assessment of perovskite sample quality.
- ItemTunable Circular Dichroism by Photoluminescent Moiré Gratings(Weinheim : Wiley-VCH, 2020) Aftenieva, Olha; Schnepf, Max; Mehlhorn, Börge; König, Tobias A.F.In nanophotonics, there is a current demand for ultrathin, flexible nanostructures that are simultaneously easily tunable, demonstrate a high contrast, and have a strong response in photoluminescent polarization. In this work, the template-assisted self-assembly of water-dispersed colloidal core–shell quantum dots into 1D light-emitting sub-micrometer gratings on a flexible substrate is demonstrated. Combining such structures with a light-absorbing metallic counterpart by simple stacking at various angles results in a tunable Moiré pattern with strong lateral contrast. Furthermore, a combination with an identical emitter-based grating leads to a chiroptical effect with a remarkably high degree of polarization of 0.72. Such a structure demonstrates direct circular polarized photoluminescence, for the first time, without a need for an additional chiral template as an intermediary. The suggested approach allows for reproducible, large-area manufacturing at reasonable costs and is of potential use for chiroptical sensors, photonic circuit applications, or preventing counterfeit. © 2020 The Authors. Advanced Optical Materials published by Wiley-VCH GmbH
- ItemRobust Single Molecule Magnet Monolayers on Graphene and Graphite with Magnetic Hysteresis up to 28 K(Weinheim : Wiley-VCH, 2021) Spree, Lukas; Liu, Fupin; Neu, Volker; Rosenkranz, Marco; Velkos, Georgios; Wang, Yaofeng; Schiemenz, Sandra; Dreiser, Jan; Gargiani, Pierluigi; Valvidares, Manuel; Chen, Chia-Hsiang; Büchner, Bernd; Avdoshenko, Stanislav M.; Popov, Alexey A.The chemical functionalization of fullerene single molecule magnet Tb2@C80(CH2Ph) enables the facile preparation of robust monolayers on graphene and highly oriented pyrolytic graphite from solution without impairing their magnetic properties. Monolayers of endohedral fullerene functionalized with pyrene exhibit magnetic bistability up to a temperature of 28 K. The use of pyrene terminated linker molecules opens the way to devise integration of spin carrying units encapsulated by fullerene cages on graphitic substrates, be it single-molecule magnets or qubit candidates. © 2021 The Authors. Advanced Functional Materials 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
- 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
- ItemSemitransparent Perovskite Solar Cells with an Evaporated Ultra-Thin Perovskite Absorber(Weinheim : Wiley-VCH, 2023) Zhang, Zongbao; Ji, Ran; Jia, Xiangkun; Wang, Shu‐Jen; Deconinck, Marielle; Siliavka, Elena; Vaynzof, YanaMetal halide perovskites are of great interest for application in semitransparent solar cells due to their tunable bandgap and high performance. However, fabricating high-efficiency perovskite semitransparent devices with high average visible transmittance (AVT) is challenging because of their high absorption coefficient. Here, a co-evaporation process is adopted to fabricate ultra-thin CsPbI3 perovskite films. The smooth surface and orientated crystal growth of the evaporated perovskite films make it possible to achieve 10 nm thin films with compact and continuous morphology without pinholes. When integrated into a p-i-n device structure of glass/ITO/PTAA/perovskite/PCBM/BCP/Al/Ag with an optimized transparent electrode, these ultra-thin layers result in an impressive open-circuit voltage (VOC) of 1.08 V and a fill factor (FF) of 80%. Consequently, a power conversion efficiency (PCE) of 3.6% with an AVT above 50% is demonstrated, which is the first report for a perovskite device of a 10 nm active layer thickness with high VOC, FF and AVT. These findings demonstrate that deposition by thermal evaporation makes it possible to form compact ultra-thin perovskite films, which are of great interest for future smart windows, light-emitting diodes, and tandem device applications.
- ItemTailoring Plasmonics of Au@Ag Nanoparticles by Silica Encapsulation(Weinheim : Wiley-VCH, 2021) Schultz, Johannes; Kirner, Felizitas; Potapov, Pavel; Büchner, Bernd; Lubk, Axel; Sturm, Elena V.Hybrid metallic nanoparticles (NPs) encapsulated in oxide shells are currently intensely studied for plasmonic applications in sensing, medicine, catalysis, and photovoltaics. Here, a method for the synthesis of Au@Ag@SiO2 cubes with a uniform silica shell of variable and adjustable thickness in the nanometer range is introduced and their excellent, highly reproducible, and tunable optical response is demonstrated. Varying the silica shell thickness, the excitation energies of the single NP plasmon modes can be tuned in a broad spectral range between 2.55 and 3.25 eV. Most importantly, a strong coherent coupling of the surface plasmons is revealed at the silver–silica interface with Mie resonances at the silica–vacuum interface leading to a significant field enhancement at the encapsulated NP surface in the range of 100% at shell thicknesses t ≃ 20 nm. Consequently, the synthesis method and the field enhancement open pathways to a widespread use of silver NPs in plasmonic applications including photonic crystals and may be transferred to other non-precious metals. © 2021 The Authors. Advanced Optical Materials published by Wiley-VCH GmbH
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