20 results
Search Results
Now showing 1 - 10 of 20
- ItemSalt concentration and charging velocity determine ion charge storage mechanism in nanoporous supercapacitors(London : Nature Publishing Group, 2018) Prehal, C.; Koczwara, C.; Amenitsch, H.; Presser, V.; Paris, O.A fundamental understanding of ion charge storage in nanoporous electrodes is essential to improve the performance of supercapacitors or devices for capacitive desalination. Here, we employ in situ X-ray transmission measurements on activated carbon supercapacitors to study ion concentration changes during electrochemical operation. Whereas counter-ion adsorption was found to dominate at small electrolyte salt concentrations and slow cycling speed, ion replacement prevails for high molar concentrations and/or fast cycling. Chronoamperometry measurements reveal two distinct time regimes of ion concentration changes. In the first regime the supercapacitor is charged, and counter- and co-ion concentration changes align with ion replacement and partially co-ion expulsion. In the second regime, the electrode charge remains constant, but the total ion concentration increases. We conclude that the initial fast charge neutralization in nanoporous supercapacitor electrodes leads to a non-equilibrium ion configuration. The subsequent, charge-neutral equilibration slowly increases the total ion concentration towards counter-ion adsorption.
- ItemSynthesis of quasi-free-standing bilayer graphene nanoribbons on SiC surfaces(London : Nature Publishing Group, 2015) Oliveira, Myriano H., Jr.; Lopes, Joao Marcelo J.; Schumann, Timo; Galves, Lauren A.; Ramsteiner, Manfred; Berlin, Katja; Trampert, Achim; Riechert, HenningScaling graphene down to nanoribbons is a promising route for the implementation of this material into devices. Quantum confinement of charge carriers in such nanostructures, combined with the electric field-induced break of symmetry in AB-stacked bilayer graphene, leads to a band gap wider than that obtained solely by this symmetry breaking. Consequently, the possibility of fabricating AB-stacked bilayer graphene nanoribbons with high precision is very attractive for the purposes of applied and basic science. Here we show a method, which includes a straightforward air annealing, for the preparation of quasi-free-standing AB-bilayer nanoribbons with different widths on SiC(0001). Furthermore, the experiments reveal that the degree of disorder at the edges increases with the width, indicating that the narrower nanoribbons are more ordered in their edge termination. In general, the reported approach is a viable route towards the large-scale fabrication of bilayer graphene nanostructures with tailored dimensions and properties for specific applications.
- ItemDirect imaging of delayed magneto-dynamic modes induced by surface acoustic waves(London : Nature Publishing Group, 2017) Foerster, Michael; Macià , Ferran; Statuto, Nahuel; Finizio, Simone; Hernández-MÃnguez, Alberto; LendÃnez, Sergi; Santos, Paulo V.; Fontcuberta, Josep; Hernà ndez, Joan Manel; Kläui, Mathias; Aballe, LuciaThe magnetoelastic effect—the change of magnetic properties caused by the elastic deformation of a magnetic material—has been proposed as an alternative approach to magnetic fields for the low-power control of magnetization states of nanoelements since it avoids charge currents, which entail ohmic losses. Here, we have studied the effect of dynamic strain accompanying a surface acoustic wave on magnetic nanostructures in thermal equilibrium. We have developed an experimental technique based on stroboscopic X-ray microscopy that provides a pathway to the quantitative study of strain waves and magnetization at the nanoscale. We have simultaneously imaged the evolution of both strain and magnetization dynamics of nanostructures at the picosecond time scale and found that magnetization modes have a delayed response to the strain modes, adjustable by the magnetic domain configuration. Our results provide fundamental insight into magnetoelastic coupling in nanostructures and have implications for the design of strain-controlled magnetostrictive nano-devices.
- ItemMapping the band structure of GeSbTe phase change alloys around the Fermi level(London : Nature Publishing Group, 2018) Kellner, J.; Bihlmayer, G.; Liebmann, M.; Otto, S.; Pauly, C.; Boschker, J.E.; Bragaglia, V.; Cecchi, S.; Wang, R.N.; Deringer, V.L.; Küppers, P.; Bhaskar, P.; Golias, E.; Sánchez-Barriga, J.; Dronskowski, R.; Fauster, T.; Rader, O.; Calarco, R.; Morgenstern, M.Phase change alloys are used for non-volatile random-access memories exploiting the conductivity contrast between amorphous and metastable, crystalline phase. However, this contrast has never been directly related to the electronic band structure. Here we employ photoelectron spectroscopy to map the relevant bands for metastable, epitaxial GeSbTe films. The constant energy surfaces of the valence band close to the Fermi level are hexagonal tubes with little dispersion perpendicular to the (111) surface. The electron density responsible for transport belongs to the tails of this bulk valence band, which is broadened by disorder, i.e., the Fermi level is 100 meV above the valence band maximum. This result is consistent with transport data of such films in terms of charge carrier density and scattering time. In addition, we find a state in the bulk band gap with linear dispersion, which might be of topological origin.
- ItemOrdered Peierls distortion prevented at growth onset of GeTe ultra-thin films(London : Nature Publishing Group, 2016) Wang, Ruining; Campi, Davide; Bernasconi, Marco; Momand, Jamo; Kooi, Bart J.; Verheijen, Marcel A.; Wuttig, Matthias; Calarco, RaffaellaUsing reflection high-energy electron diffraction (RHEED), the growth onset of molecular beam epitaxy (MBE) deposited germanium telluride (GeTe) film on Si(111)-(√3 × √3)R30°-Sb surfaces is investigated, and a larger than expected in-plane lattice spacing is observed during the deposition of the first two molecular layers. High-resolution transmission electron microscopy (HRTEM) confirms that the growth proceeds via closed layers, and that those are stable after growth. The comparison of the experimental Raman spectra with theoretical calculated ones allows assessing the shift of the phonon modes for a quasi-free-standing ultra-thin GeTe layer with larger in-plane lattice spacing. The manifestation of the latter phenomenon is ascribed to the influence of the interface and the confinement of GeTe within the limited volume of material available at growth onset, either preventing the occurrence of Peierls dimerization or their ordered arrangement to occur normally.
- ItemEfficient synthesis of triarylamine-based dyes for p-type dye-sensitized solar cells(London : Nature Publishing Group, 2016) Wild, Martin; Griebel, Jan; Hajduk, Anna; Friedrich, Dirk; Stark, Annegret; Abel, Bernd; Siefermann, Katrin R.The class of triarylamine-based dyes has proven great potential as efficient light absorbers in inverse (p-type) dye sensitized solar cells (DSSCs). However, detailed investigation and further improvement of p-type DSSCs is strongly hindered by the fact that available synthesis routes of triarylamine-based dyes are inefficient and particularly demanding with regard to time and costs. Here, we report on an efficient synthesis strategy for triarylamine-based dyes for p-type DSSCs. A protocol for the synthesis of the dye-precursor (4-(bis(4-bromophenyl)amino)benzoic acid) is presented along with its X-ray crystal structure. The dye precursor is obtained from the commercially available 4(diphenylamino)benzaldehyde in a yield of 87% and serves as a starting point for the synthesis of various triarylamine-based dyes. Starting from the precursor we further describe a synthesis protocol for the dye 4-{bis[4′-(2,2-dicyanovinyl)-[1,1′-biphenyl]-4-yl]amino}benzoic acid (also known as dye P4) in a yield of 74%. All synthesis steps are characterized by high yields and high purities without the need for laborious purification steps and thus fulfill essential requirements for scale-up.
- ItemObservation of T2-like coherent optical phonons in epitaxial Ge2Sb2Te5/GaSb(001) films(London : Nature Publishing Group, 2013) Shalini, A.; Liu, Y.; Al-Jarah, U.A.S.; Srivastava, G.P.; Wright, C.D.; Katmis, F.; Braun, W.; Hicken, R.J.The phonon spectrum of Ge2Sb2Te5 is a signature of its crystallographic structure and underlies the phase transition process used in memory applications. Epitaxial materials allow coherent optical phonons to be studied in femtosecond anisotropic reflectance measurements. A dominant phonon mode with frequency of 3.4 THz has been observed in epitaxial Ge2Sb2Te5 grown on GaSb(001). The dependence of signal strength upon pump and probe polarization is described by a theory of transient stimulated Raman scattering that accounts for the symmetry of the crystallographic structure through use of the Raman tensor. The 3.4 THz mode has the character of the 3 dimensional T2 mode expected for the Oh point group, confirming that the underlying crystallographic structure is cubic. New modes are observed in both Ge2Sb2Te5 and GaSb after application of large pump fluences, and are interpreted as 1 and 2 dimensional modes associated with segregation of Sb.
- ItemFar-infrared and Raman spectroscopy investigation of phonon modes in amorphous and crystalline epitaxial GeTe-Sb2Te3 alloys(London : Nature Publishing Group, 2016) Bragaglia, V.; Holldack, K.; Boschker, J.E.; Arciprete, F.; Zallo, E.; Flissikowski, T.; Calarco, R.A combination of far-infrared and Raman spectroscopy is employed to investigate vibrational modes and the carrier behavior in amorphous and crystalline ordered GeTe-Sb2Te3 alloys (GST) epitaxially grown on Si(111). The infrared active GST mode is not observed in the Raman spectra and vice versa, indication of the fact that inversion symmetry is preserved in the metastable cubic phase in accordance with the Fm3 space group. For the trigonal phase, instead, a partial symmetry break due to Ge/Sb mixed anion layers is observed. By studying the crystallization process upon annealing with both the techniques, we identify temperature regions corresponding to the occurrence of different phases as well as the transition from one phase to the next. Activation energies of 0.43 eV and 0.08 eV for the electron conduction are obtained for both cubic and trigonal phases, respectively. In addition a metal-insulator transition is clearly identified to occur at the onset of the transition between the disordered and the ordered cubic phase.
- ItemA hybrid MBE-based growth method for large-area synthesis of stacked hexagonal boron nitride/graphene heterostructures(London : Nature Publishing Group, 2017) Wofford, Joseph M.; Nakhaie, Siamak; Krause, Thilo; Liu, Xianjie; Ramsteiner, Manfred; Hanke, Michael; Riechert, Henning; Lopes, J.; Marcelo, J.Van der Waals heterostructures combining hexagonal boron nitride (h-BN) and graphene offer many potential advantages, but remain difficult to produce as continuous films over large areas. In particular, the growth of h-BN on graphene has proven to be challenging due to the inertness of the graphene surface. Here we exploit a scalable molecular beam epitaxy based method to allow both the h-BN and graphene to form in a stacked heterostructure in the favorable growth environment provided by a Ni(111) substrate. This involves first saturating a Ni film on MgO(111) with C, growing h-BN on the exposed metal surface, and precipitating the C back to the h-BN/Ni interface to form graphene. The resulting laterally continuous heterostructure is composed of a top layer of few-layer thick h-BN on an intermediate few-layer thick graphene, lying on top of Ni/MgO(111). Examinations by synchrotron-based grazing incidence diffraction, X-ray photoemission spectroscopy, and UV-Raman spectroscopy reveal that while the h-BN is relaxed, the lattice constant of graphene is significantly reduced, likely due to nitrogen doping. These results illustrate a different pathway for the production of h-BN/graphene heterostructures, and open a new perspective for the large-area preparation of heterosystems combining graphene and other 2D or 3D materials.
- ItemRole of interfaces on the stability and electrical properties of Ge2Sb2Te5 crystalline structures(London : Nature Publishing Group, 2017) Mio, A.M.; Privitera, S.M.S.; Bragaglia, V.; Arciprete, F.; Cecchi, S.; Litrico, G.; Persch, C.; Calarco, R.; Rimini, E.GeSbTe-based materials exhibit multiple crystalline phases, from disordered rocksalt, to rocksalt with ordered vacancy layers, and to the stable trigonal phase. In this paper we investigate the role of the interfaces on the structural and electrical properties of Ge2Sb2Te5. We find that the site of nucleation of the metastable rocksalt phase is crucial in determining the evolution towards vacancy ordering and the stable phase. By properly choosing the substrate and the capping layers, nucleation sites engineering can be obtained, thus promoting or preventing the vacancy ordering in the rocksalt structure or the conversion into the trigonal phase. The vacancy ordering occurs at lower annealing temperatures (170 °C) for films deposited in the amorphous phase on silicon (111), compared to the case of SiO2 substrate (200 °C), or in presence of a capping layer (330 °C). The mechanisms governing the nucleation have been explained in terms of interfacial energies. Resistance variations of about one order of magnitude have been measured upon transition from the disordered to the ordered rocksalt structure and then to the trigonal phase. The possibility to control the formation of the crystalline phases characterized by marked resistivity contrast is of fundamental relevance for the development of multilevel phase change data storage.