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- ItemFulleretic well-defined scaffolds: Donor–fullerene alignment through metal coordination and its effect on photophysics(Hoboken, NJ : Wiley, 2016) Williams, Derek E.; Dolgopolova, Ekaterina A.; Godfrey, Danielle C.; Ermolaeva, Evgeniya D.; Pellechia, Perry J.; Greytak, Andrew B.; Smith, Mark D.; Avdoshenko, Stanislav M.; Popov, Alexey A.; Shustova, Natalia B.Herein, we report the first example of a crystalline metal–donor–fullerene framework, in which control of the donor–fullerene mutual orientation was achieved through chemical bond formation, in particular, by metal coordination. The 13C cross‐polarization magic‐angle spinning NMR spectroscopy, X‐ray diffraction, and time‐resolved fluorescence spectroscopy were performed for comprehensive structural analysis and energy‐transfer (ET) studies of the fulleretic donor–acceptor scaffold. Furthermore, in combination with photoluminescence measurements, the theoretical calculations of the spectral overlap function, Förster radius, excitation energies, and band structure were employed to elucidate the photophysical and ET processes in the prepared fulleretic material. We envision that the well‐defined fulleretic donor–acceptor materials could contribute not only to the basic science of fullerene chemistry but would also be used towards effective development of organic photovoltaics and molecular electronics.
- ItemRoles of hydrogenation, annealing and field in the structure and magnetic entropy change of Tb-based bulk metallic glasses(New York : American Institute of Physics, 2013) Luo, Qiang; Schwarz, Björn; Mattern, Norbert; Shen, Jun; Eckert, JürgenThe reduction of open-volume regions in Tb-based metallic glass (MG) by annealing and hydrogen charging was found to rearrange the atomic structure and tune the magnetic behaviors. After crystallization, the magnetic structure and magnetic entropy change (MEC) alters due to the structural transformation, and a plateau-like-MEC behavior can be obtained. The hydrogen concentration after charging at 1mA/cm2 for 576 h reaches as high as 3290 w-ppm. The magnetization behavior and the MEC change due to the modification of the exchange interaction and the random magnetic anisotropy (RMA) upon hydrogenation. At low temperatures, irreversible positive MEC was obtained, which is related to the internal entropy production. The RMA-to-exchange ratio acts as a switch to control the irreversible entropy production channel and the reversible entropy transfer channel. The field dependence of the MEC is discussed in term of the competition among Zeeman energy, exchange interaction and RMA.
- ItemPronounced ductility in CuZrAl ternary bulk metallic glass composites with optimized microstructure through melt adjustment(New York : American Institute of Physics, 2012) Liu, Zengqian; Li, Ran; Liu, Gang; Song, Kaikai; Pauly, Simon; Zhang, Tao; Eckert, JürgenMicrostructures and mechanical properties of as-cast Cu47.5Zr47.5Al5 bulk metallic glass composites are optimized by appropriate remelting treatment of master alloys. With increasing remelting time, the alloys exhibit homogenized size and distribution of in situ formed B2 CuZr crystals. Pronounced tensile ductility of ∼13.6% and work-hardening ability are obtained for the composite with optimized microstructure. The effect of remelting treatment is attributed to the suppressed heterogeneous nucleation and growth of the crystalline phase from undercooled liquid, which may originate from the dissolution of oxides and nitrides as well as from the micro-scale homogenization of the melt.
- ItemStimuli‐responsive microjets with reconfigurable shape(Hoboken, NJ : Wiley, 2014) Magdanz, Veronika; Stoychev, Georgi; Ionov, Leonid; Sanchez, Samuel; Schmidt, Oliver.G.Flexible thermoresponsive polymeric microjets are formed by the self‐folding of polymeric layers containing a thin Pt film used as catalyst for self‐propulsion in solutions containing hydrogen peroxide. The flexible microjets can reversibly fold and unfold in an accurate manner by applying changes in temperature to the solution in which they are immersed. This effect allows microjets to rapidly start and stop multiple times by controlling the radius of curvature of the microjet. This work opens many possibilities in the field of artificial nanodevices, for fundamental studies on self‐propulsion at the microscale, and also for biorelated applications.
- ItemHigh-performance Li-O2 batteries with trilayered Pd/MnOx/Pd nanomembranes(Hoboken, NJ : Wiley, 2015) Lu, Xueyi; Deng, Junwen; Si, Wenping; Sun, Xiaolei; Liu, Xianghong; Liu, Bo; Liu, Lifeng; Oswald, Steffen; Baunack, Stefan; Grafe, Hans Joachim; Yan, Chenglin; Schmidt, Oliver G.Trilayered Pd/MnOx/Pd nanomembranes are fabricated as the cathode catalysts for Li‐O2 batteries. The combination of Pd and MnOx facilitates the transport of electrons, lithium ions, and oxygen‐containing intermediates, thus effectively decomposing the discharge product Li2O2 and significantly lowering the charge overpotential and enhancing the power efficiency. This is promising for future environmentally friendly applications.
- ItemCorrelation between the microstructures and the deformation mechanisms of CuZr-based bulk metallic glass composites(New York : American Institute of Physics, 2013) Song, K.K.; Pauly, S.; Sun, B.A; Tan, J.; Stoica, M.; Kühn, U.; Eckert, J.The variation of the transformation-mediated deformation behavior with microstructural changes in CuZr-based bulk metallic glass composites is investigated. With increasing crystalline volume fraction, the deformation mechanism gradually changes from a shear-banding dominated process as evidenced by a chaotic serrated flow behavior, to being governed by a martensitic transformation with a pronounced elastic-plastic stage, resulting in different plastic deformations evolving into a self-organized critical state characterized by the power-law distribution of shear avalanches. This is reflected in the stress-strain curves by a single-to-"double"-to-"triple"- double yielding transition and by different mechanical properties with different serrated flow characteristics, which are interpreted based on the microstructural evolutions and a fundamental energy theorem. Our results can assist in understanding deformation behaviors for high-performance metastable alloys.
- ItemThe influence of the in-plane lattice constant on the superconducting transition temperature of FeSe0.7Te0.3 thin films(New York : American Institute of Physics, 2017) Yuan, Feifei; Iida, Kazumasa; Grinenko, Vadim; Chekhonin, Paul; Pukenas, Aurimas; Skrotzki, Werner; Sakoda, Masahito; Naito, Michio; Sala, Alberto; Putti, Marina; Yamashita, Aichi; Takano, Yoshihiko; Shi, Zhixiang; Nielsch, Kornelius; Hühne, RubenEpitaxial Fe(Se,Te) thin films were prepared by pulsed laser deposition on (La0.18Sr0.82)(Al0.59Ta0.41)O3 (LSAT), CaF2-buffered LSAT and bare CaF2 substrates, which exhibit an almost identical in-plane lattice parameter. The composition of all Fe(Se,Te) films were determined to be FeSe0.7Te0.3 by energy dispersive X-ray spectroscopy, irrespective of the substrate. Albeit the lattice parameters of all templates have comparable values, the in-plane lattice parameter of the FeSe0.7Te0.3 films varies significantly. We found that the superconducting transition temperature (Tc) of FeSe0.7Te0.3 thin films is strongly correlated with their a-axis lattice parameter. The highest Tc of over 19 K was observed for the film on bare CaF2 substrate, which is related to unexpectedly large in-plane compressive strain originating mostly from the thermal expansion mismatch between the FeSe0.7Te0.3 film and the substrate.
- ItemControllable sliding transfer of wafer‐size graphene(Hoboken, NJ : Wiley, 2016) Lu, Wenjing; Zeng, Mengqi; Li, Xuesong; Wang, Jiao; Tan, Lifang; Shao, Miaomiao; Han, Jiangli; Wang, Sheng; Yue, Shuanglin; Zhang, Tao; Hu, Xuebo; Mendes, Rafael G.; Rümmeli, Mark H.; Peng, Lianmao; Liu, Zhongfan; Fu, LeiThe innovative design of sliding transfer based on a liquid substrate can succinctly transfer high‐quality, wafer‐size, and contamination‐free graphene within a few seconds. Moreover, it can be extended to transfer other 2D materials. The efficient sliding transfer approach can obtain high‐quality and large‐area graphene for fundamental research and industrial applications.
- ItemCeria/silicon carbide core–shell materials prepared by miniemulsion technique(Frankfurt, M. : Beilstein-Institut zur Förderung der Chemischen Wissenschaften, 2011) Borchardt, Lars; Oschatz, Martin; Frind, Robert; Kockrick, Emanuel; Lohe, Martin R.; Hauser, Christoph P.; Weiss, Clemens K.; Landfester, Katharina; Büchner, Bernd; Kaskel, StefanFor the first time we present the synthesis of CeO2/Si(O)C core–shell particles prepared by the miniemulsion technique. The Si(O)C core was obtained by means of a polycarbosilane precursor (SMP10), which was subsequently functionalized with ceria and pyrolyzed to the ceramic. The size of these particles could easily be adjusted by varying the surfactants and the surfactant concentration, or by the addition of comonomers. Hence particle sizes ranged from 100 to 1000 nm, tunable by the preparation conditions. All materials were characterized by photon cross correlation spectroscopy, scanning electron microscopy and elemental mapping investigations. Furthermore, first catalytic tests were carried out by temperature programmed oxidation (TPO) of methane, and the activity of this material in lowering the onset temperature of methane combustion by 262 K was documented.
- ItemInfluence of grain size and composition, topology and excess free volume on the deformation behavior of Cu–Zr nanoglasses(Frankfurt, M. : Beilstein-Institut zur Förderung der Chemischen Wissenschaften, 2015) Şopu, Daniel; Albe, KarstenThe influence of grain size and composition on the mechanical properties of Cu–Zr nanoglasses (NGs) is investigated by molecular dynamics simulations using two model glasses of different alloy composition, namely Cu64Zr36 (Cu-rich) and Cu36Zr64 (Zr-rich). When the grain size is increased, or the fraction of interfaces in these NGs is decreased, we find a transition from a homogeneous to an inhomogeneous plastic deformation, because the softer interfaces are promoting the formation shear transformation zones. In case of the Cu-rich system, shear localization at the interfaces is most pronounced, since both the topological order and free volume content of the interfaces are very different from the bulk phase. After thermal treatment the redistribution of free volume leads to a more homogenous deformation behavior. The deformation behavior of the softer Zr-rich nanoglass, in contrast, is only weakly affected by the presence of glass–glass interfaces, since the interfaces don’t show topological disorder. Our results provide clear evidence that the mechanical properties of metallic NGs can be systematically tuned by controlling the size and the chemical composition of the glassy nanograins.