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Fulleretic well-defined scaffolds: Donor–fullerene alignment through metal coordination and its effect on photophysics

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.

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Stimuli‐responsive microjets with reconfigurable shape

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.

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The influence of the in-plane lattice constant on the superconducting transition temperature of FeSe0.7Te0.3 thin films

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, Ruben

Epitaxial 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.

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Tuning the spin coherence time of Cu(II)−(bis)oxamato and Cu(II)−(bis)oxamidato complexes by advanced ESR pulse protocols

2017-4-27, Zaripov, Ruslan, Vavilova, Evgeniya, Khairuzhdinov, Iskander, Salikhov, Kev, Voronkova, Violeta, Abdulmalic, Mohammad A., Meva, Francois E., Weheabby, Saddam, Rüffer, Tobias, Büchner, Bernd, Kataev, Vladislav

We have investigated with the pulsed ESR technique at X- and Q-band frequencies the coherence and relaxation of Cu spins S = 1/2 in single crystals of diamagnetically diluted mononuclear [n-Bu4N]2[Cu(opba)] (1%) in the host lattice of [n-Bu4N]2[Ni(opba)] (99%, opba = o-phenylenebis(oxamato)) and of diamagnetically diluted mononuclear [n-Bu4N]2[Cu(opbon-Pr2)] (1%) in the host lattice of [n-Bu4N]2[Ni(opbon-Pr2)] (99%, opbon-Pr2 = o-phenylenebis(N(propyl)oxamidato)). For that we have measured the electron spin dephasing time Tm at different temperatures with the two-pulse primary echo and with the special Carr–Purcell–Meiboom–Gill (CPMG) multiple microwave pulse sequence. Application of the CPMG protocol has led to a substantial increase of the spin coherence lifetime in both complexes as compared to the primary echo results. It shows the efficiency of the suppression of the electron spin decoherence channel in the studied complexes arising due to spectral diffusion induced by a random modulation of the hyperfine interaction with the nuclear spins. We argue that this method can be used as a test for the relevance of the spectral diffusion for the electron spin decoherence. Our results have revealed a prominent role of the opba4– and opbon-Pr24– ligands for the dephasing of the Cu spins. The presence of additional 14N nuclei and protons in [Cu(opbon-Pr2)]2– as compared to [Cu(opba)]2– yields significantly shorter Tm times. Such a detrimental effect of the opbon-Pr24− ligands has to be considered when discussing a potential application of the Cu(II)−(bis)oxamato and Cu(II)−(bis)oxamidato complexes as building blocks of more complex molecular structures in prototype spintronic devices. Furthermore, in our work we propose an improved CPMG pulse protocol that enables elimination of unwanted echoes that inevitably appear in the case of inhomogeneously broadened ESR spectra due to the selective excitation of electron spins.

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Roles of hydrogenation, annealing and field in the structure and magnetic entropy change of Tb-based bulk metallic glasses

2013, Luo, Qiang, Schwarz, Björn, Mattern, Norbert, Shen, Jun, Eckert, Jürgen

The 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.

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High-performance Li-O2 batteries with trilayered Pd/MnOx/Pd nanomembranes

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.

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Electrically-Pumped Wavelength-Tunable GaAs Quantum Dots Interfaced with Rubidium Atoms

2017, Huang, Huiying, Trotta, Rinaldo, Huo, Yongheng, Lettner, Thomas, Wildmann, Johannes S., Martín-Sánchez, Javier, Huber, Daniel, Reindl, Marcus, Zhang, Jiaxiang, Zallo, Eugenio, Schmidt, Oliver G., Rastelli, Armando

We demonstrate the first wavelength-tunable electrically pumped source of nonclassical light that can emit photons with wavelength in resonance with the D2 transitions of 87Rb atoms. The device is fabricated by integrating a novel GaAs single-quantum-dot light-emitting diode (LED) onto a piezoelectric actuator. By feeding the emitted photons into a 75 mm long cell containing warm 87Rb vapor, we observe slow-light with a temporal delay of up to 3.4 ns. In view of the possibility of using 87Rb atomic vapors as quantum memories, this work makes an important step toward the realization of hybrid-quantum systems for future quantum networks.

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Pronounced ductility in CuZrAl ternary bulk metallic glass composites with optimized microstructure through melt adjustment

2012, Liu, Zengqian, Li, Ran, Liu, Gang, Song, Kaikai, Pauly, Simon, Zhang, Tao, Eckert, Jürgen

Microstructures 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.

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Correlation between the microstructures and the deformation mechanisms of CuZr-based bulk metallic glass composites

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.

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Controllable sliding transfer of wafer‐size graphene

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, Lei

The 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.