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- ItemA High-Voltage, Dendrite-Free, and Durable Zn–Graphite Battery(Weinheim : Wiley-VCH, 2019) Wang, Gang; Kohn, Benjamin; Scheler, Ulrich; Wang, Faxing; Oswald, Steffen; Löffler, Markus; Tan, Deming; Zhang, Panpan; Zhang, Jian; Feng, XinliangThe intrinsic advantages of metallic Zn, like high theoretical capacity (820 mAh g−1), high abundance, low toxicity, and high safety have driven the recent booming development of rechargeable Zn batteries. However, the lack of high-voltage electrolyte and cathode materials restricts the cell voltage mostly to below 2 V. Moreover, dendrite formation and the poor rechargeability of the Zn anode hinder the long-term operation of Zn batteries. Here a high-voltage and durable Zn–graphite battery, which is enabled by a LiPF6-containing hybrid electrolyte, is reported. The presence of LiPF6 efficiently suppresses the anodic oxidation of Zn electrolyte and leads to a super-wide electrochemical stability window of 4 V (vs Zn/Zn2+). Both dendrite-free Zn plating/stripping and reversible dual-anion intercalation into the graphite cathode are realized in the hybrid electrolyte. The resultant Zn–graphite battery performs stably at a high voltage of 2.8 V with a record midpoint discharge voltage of 2.2 V. After 2000 cycles at a high charge–discharge rate, high capacity retention of 97.5% is achieved with ≈100% Coulombic efficiency. © 2019 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
- ItemPAH/PAH(CF3)n Donor/Acceptor Charge-Transfer Complexes in Solution and in Solid-State Co-Crystals(Weinheim : Wiley-VCH, 2019) Castro, Karlee P.; Bukovsky, Eric V.; Kuvychko, Igor V.; DeWeerd, Nicholas J.; Chen, Yu-Sheng; Deng, Shihu H.M.; Wang, Xue-Bin; Popov, Alexey A.; Strauss, Steven H.; Boltalina, Olga V.A solution, solid-state, and computational study is reported of polycyclic aromatic hydrocarbon PAH/PAH(CF3)n donor/acceptor (D/A) charge-transfer complexes that involve six PAH(CF3)n acceptors with known gas-phase electron affinities that range from 2.11(2) to 2.805(15) eV and four PAH donors, including seven CT co-crystal X-ray structures that exhibit hexagonal arrays of mixed π-stacks with 1/1, 1/2, or 2/1 D/A stoichiometries (PAH=anthracene, azulene, coronene, perylene, pyrene, triphenylene; n=5, 6). These are the first D/A CT complexes with PAH(CF3)n acceptors to be studied in detail. The nine D/A combinations were chosen to allow several structural and electronic comparisons to be made, providing new insights about controlling D/A interactions and the structures of CT co-crystals. The comparisons include, among others, CT complexes of the same PAH(CF3)n acceptor with four PAH donors and CT complexes of the same donor with four PAH(CF3)n acceptors. All nine CT complexes exhibit charge-transfer bands in solution with λmax between 467 and 600 nm. A plot of E(λmax) versus [IE(donor)−EA(acceptor)] for the nine CT complexes studied is linear with a slope of 0.72±0.03 eV eV−1. This plot is the first of its kind for CT complexes with structurally related donors and acceptors for which precise experimental gas-phase IEs and EAs are known. It demonstrates that conclusions based on the common assumption that the slope of a CT E(λmax) versus [IE−EA] plot is unity may be incorrect in at least some cases and should be reconsidered. © 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
- ItemIndependent Geometrical Control of Spin and Charge Resistances in Curved Spintronics(Washington, DC : ACS Publ., 2019) Das, Kumar Sourav; Makarov, Denys; Gentile, Paola; Cuoco, Mario; Van Wees, Bart J.; Ortix, Carmine; Vera-Marun, Ivan J.Spintronic devices operating with pure spin currents represent a new paradigm in nanoelectronics, with a higher energy efficiency and lower dissipation as compared to charge currents. This technology, however, will be viable only if the amount of spin current diffusing in a nanochannel can be tuned on demand while guaranteeing electrical compatibility with other device elements, to which it should be integrated in high-density three-dimensional architectures. Here, we address these two crucial milestones and demonstrate that pure spin currents can effectively propagate in metallic nanochannels with a three-dimensional curved geometry. Remarkably, the geometric design of the nanochannels can be used to reach an independent tuning of spin transport and charge transport characteristics. These results laid the foundation for the design of efficient pure spin current-based electronics, which can be integrated in complex three-dimensional architectures. © 2019 American Chemical Society.
- ItemDirect Observation of Plasmon Band Formation and Delocalization in Quasi-Infinite Nanoparticle Chains(Washington, DC : ACS Publ., 2019) Mayer, Martin; Potapov, Pavel L.; Pohl, Darius; Steiner, Anja Maria; Schultz, Johannes; Rellinghaus, Bernd; Lubk, Axel; König, Tobias A.F.; Fery, AndreasChains of metallic nanoparticles sustain strongly confined surface plasmons with relatively low dielectric losses. To exploit these properties in applications, such as waveguides, the fabrication of long chains of low disorder and a thorough understanding of the plasmon-mode properties, such as dispersion relations, are indispensable. Here, we use a wrinkled template for directed self-assembly to assemble chains of gold nanoparticles. With this up-scalable method, chain lengths from two particles (140 nm) to 20 particles (1500 nm) and beyond can be fabricated. Electron energy-loss spectroscopy supported by boundary element simulations, finite-difference time-domain, and a simplified dipole coupling model reveal the evolution of a band of plasmonic waveguide modes from degenerated single-particle modes in detail. In striking difference from plasmonic rod-like structures, the plasmon band is confined in excitation energy, which allows light manipulations below the diffraction limit. The non-degenerated surface plasmon modes show suppressed radiative losses for efficient energy propagation over a distance of 1500 nm. © 2019 American Chemical Society.
- ItemThree-Dimensional Superconducting Nanohelices Grown by He+-Focused-Ion-Beam Direct Writing(Washington, DC : ACS Publ., 2019) Córdoba, Rosa; Mailly, Dominique; Rezaev, Roman O.; Smirnova, Ekaterina I.; Schmidt, Oliver G.; Fomin, Vladimir M.; Zeitler, Uli; Guillamón, Isabel; Suderow, Hermann; De Teresa, José MaríaNovel schemes based on the design of complex three-dimensional (3D) nanoscale architectures are required for the development of the next generation of advanced electronic components. He+ focused-ion-beam (FIB) microscopy in combination with a precursor gas allows one to fabricate 3D nanostructures with an extreme resolution and a considerably higher aspect ratio than FIB-based methods, such as Ga+ FIB-induced deposition, or other additive manufacturing technologies. In this work, we report the fabrication of 3D tungsten carbide nanohelices with on-demand geometries via controlling key deposition parameters. Our results show the smallest and highest-densely packed nanohelix ever fabricated so far, with dimensions of 100 nm in diameter and aspect ratio up to 65. These nanohelices become superconducting at 7 K and show a large critical magnetic field and critical current density. In addition, given its helical 3D geometry, fingerprints of vortex and phase-slip patterns are experimentally identified and supported by numerical simulations based on the time-dependent Ginzburg-Landau equation. These results can be understood by the helical geometry that induces specific superconducting properties and paves the way for future electronic components, such as sensors, energy storage elements, and nanoantennas, based on 3D compact nanosuperconductors. © 2019 American Chemical Society.
- ItemThe influence of partial replacement of Cu with Ga on the corrosion behavior of Ti40Zr10Cu36PD14 metallic glasses(Bristol : IOP Publishing, 2019) Wei, Qi; Gostin, Petre Flaviu; Addison, Owen; Reed, Daniel; Calin, Mariana; Bera, Supriya; Ramasamy, Parthiban; Davenport, AlisonTiZrCuPdGa metallic glasses are under consideration for small dental biomedical implants. There is interest in replacing some of the Cu with Ga to improve the glass-forming ability and biocompatibility. Ti40Zr10Cu36-xPd14Gax (x = 0, 1, 2, 4, 8 and 10 at.%) metallic glasses in rod and ribbon forms were fabricated by mould casting and melt spinning, respectively, and electrochemically tested in a 0.9wt.% NaCl (0.154 M) solution. It has been shown that for both rod and ribbon samples Ga levels up to 8% have no significant effect on passive current density, pitting potential or cathodic reactivity in 0.9% NaCl at 37°C. Different pitting potential and corrosion potential values were found when ribbon and rod samples of the same composition were compared for all compositions apart from the one containing the highest Ga level (10%). This was attributed to structural relaxation occurring as a result of the slower cooling rates during casting rods compared with melt-spinning ribbons. Substitution of Ga for Cu in these metallic glasses therefore expected to have no significant effect on corrosion susceptibility. © The Author(s) 2019.
- ItemThe Effect of Boron Content on Wetting Kinetics in Si-B Alloy/h-BN System(New York, NY : Springer, 2019) Polkowski, Wojciech; Sobczak, Natalia; Bruzda, Grzegorz; Nowak, Rafał; Giuranno, Donatella; Kudyba, Artur; Polkowska, Adelajda; Pajor, Krzysztof; Kozieł, Tomasz; Kaban, IvanIn this work, the effect of boron content on the high-temperature wetting behavior in the Si-B alloy/h-BN systems was experimentally examined. For this reason, hypoeutectic, eutectic and hypereutectic Si-B alloys (Si-1B, Si-3.2B and Si-5.7B wt.%, respectively) were produced by electric arc melting method and then subjected to sessile drop/contact heating experiments with polycrystalline h-BN substrates, at temperatures up to 1750 °C. Similar to pure Si/h-BN system, wetting kinetics curves calculated on a basis of in situ recorded drop/substrate images point toward non-wetting behavior of all selected Si-B alloy/h-BN couples. The highest contact angle values of ~ 150° were obtained for hypoeutectic and eutectic Si-B alloys in the whole examined temperature range. © 2018, The Author(s).
- ItemHigh-Temperature Interaction of Liquid Gd with Y2O3(New York, NY : Springer, 2019) Turalska, P.; Sobczak, N.; Bruzda, G.; Kaban, I.; Mattern, N.The sessile drop method combined with contact heating procedure was applied for the investigation of high-temperature interaction between liquid Gd and Y2O3 substrate. Real-time behavior of Gd sample in flowing inert gas (Ar) atmosphere upon heating to and at temperature of 1362 °C was recorded using high-speed high-resolution CCD camera. The results evidenced that molten Gd wets Y2O3 substrate (the contact angle θ < 90°) immediately after melting of metal sample observed at T = 1324 °C (Tm = 1312 °C). During the first 3 min of the sessile drop test, the contact angle dropped from θ = 52° to θ = 24° and then stabilized at the final value of θf * = 33°. The solidified Gd/Y2O3 couple was subjected to structural characterization using optical microscopy, scanning electron microscopy coupled with x-ray energy-dispersive spectroscopy. The results evidenced that the wettability in the Gd/Y2O3 system has a reactive nature and the leading mechanism of the interaction between liquid Gd and Y2O3 is the dissolution of the ceramic in the liquid metal responsible for the formation of a deep crater in the substrate under the drop. Therefore, the final contact angle θf*, estimated from the side-view drop image, should be considered as an apparent value, compared to the more reliable value of θf = 70° measured on the cross section of the solidified couple. © 2019, The Author(s).
- ItemNanomagnetism of Magnetoelectric Granular Thin-Film Antiferromagnets(Washington, DC : ACS Publ., 2019) Appel, Patrick; Shields, Brendan J.; Kosub, Tobias; Hedrich, Natascha; Hübner, René; Faßbender, Jürgen; Makarov, Denys; Maletinsky, PatrickAntiferromagnets have recently emerged as attractive platforms for spintronics applications, offering fundamentally new functionalities compared with their ferromagnetic counterparts. Whereas nanoscale thin-film materials are key to the development of future antiferromagnetic spintronic technologies, existing experimental tools tend to suffer from low resolution or expensive and complex equipment requirements. We offer a simple, high-resolution alternative by addressing the ubiquitous surface magnetization of magnetoelectric antiferromagnets in a granular thin-film sample on the nanoscale using single-spin magnetometry in combination with spin-sensitive transport experiments. Specifically, we quantitatively image the evolution of individual nanoscale antiferromagnetic domains in 200 nm thin films of Cr 2 O 3 in real space and across the paramagnet-to-antiferromagnet phase transition, finding an average domain size of 230 nm, several times larger than the average grain size in the film. These experiments allow us to discern key properties of the Cr 2 O 3 thin film, including the boundary magnetic moment density, the variation of critical temperature throughout the film, the mechanism of domain formation, and the strength of exchange coupling between individual grains comprising the film. Our work offers novel insights into the magnetic ordering mechanism of Cr 2 O 3 and firmly establishes single-spin magnetometry as a versatile and widely applicable tool for addressing antiferromagnetic thin films on the nanoscale. © 2019 American Chemical Society.