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- 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.
- 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.
- ItemSuperconducting ferecrystals: Turbostratically disordered atomic-scale layered (PbSe)1.14(NbSe2)n thin films(London : Nature Publishing Group, 2016) Grosse, Corinna; Alemayehu, Matti B.; Falmbigl, Matthias; Mogilatenko, Anna; Chiatti, Olivio; Johnson, David C.; Fischer, Saskia F.Hybrid electronic heterostructure films of semi- and superconducting layers possess very different properties from their bulk counterparts. Here, we demonstrate superconductivity in ferecrystals: turbostratically disordered atomic-scale layered structures of single-, bi- and trilayers of NbSe2 separated by PbSe layers. The turbostratic (orientation) disorder between individual layers does not destroy superconductivity. Our method of fabricating artificial sequences of atomic-scale 2D layers, structurally independent of their neighbours in the growth direction, opens up new possibilities of stacking arbitrary numbers of hybrid layers which are not available otherwise, because epitaxial strain is avoided. The observation of superconductivity and systematic Tc changes with nanostructure make this synthesis approach of particular interest for realizing hybrid systems in the search of 2D superconductivity and the design of novel electronic heterostructures.
- ItemCrystallization of Ge2Sb2Te5 thin films by nano- and femtosecond single laser pulse irradiation(London : Nature Publishing Group, 2016) Sun, Xinxing; Ehrhardt, Martin; Lotnyk, Andriy; Lorenz, Pierre; Thelander, Erik; Gerlach, Jürgen W.; Smausz, Tomi; Decker, Ulrich; Rauschenbach, BerndThe amorphous to crystalline phase transformation of Ge2Sb2Te5 (GST) films by UV nanosecond (ns) and femtosecond (fs) single laser pulse irradiation at the same wavelength is compared. Detailed structural information about the phase transformation is collected by x-ray diffraction and high resolution transmission electron microscopy (TEM). The threshold fluences to induce crystallization are determined for both pulse lengths. A large difference between ns and fs pulse irradiation was found regarding the grain size distribution and morphology of the crystallized films. For fs single pulse irradiated GST thin films, columnar grains with a diameter of 20 to 60 nm were obtained as evidenced by cross-sectional TEM analysis. The local atomic arrangement was investigated by highresolution Cs-corrected scanning TEM. Neither tetrahedral nor off-octahedral positions of Ge-atoms could be observed in the largely defect-free grains. A high optical reflectivity contrast (~25%) between amorphous and completely crystallized GST films was achieved by fs laser irradiation induced at fluences between 13 and 16 mJ/cm2 and by ns laser irradiation induced at fluences between 67 and 130 mJ/cm2. Finally, the fluence dependent increase of the reflectivity is discussed in terms of each photon involved into the crystallization process for ns and fs pulses, respectively.
- ItemMetal - Insulator transition driven by vacancy ordering in GeSbTe phase change materials(London : Nature Publishing Group, 2016) Bragaglia, Valeria; Arciprete, Fabrizio; Zhang, Wei; Mio, Antonio Massimiliano; Zallo, Eugenio; Perumal, Karthick; Giussani, Alessandro; Cecchi, Stefano; Boschker, Jos Emiel; Riechert, Henning; Privitera, Stefania; Rimini, Emanuele; Mazzarello, Riccardo; Calarco, RaffaellaPhase Change Materials (PCMs) are unique compounds employed in non-volatile random access memory thanks to the rapid and reversible transformation between the amorphous and crystalline state that display large differences in electrical and optical properties. In addition to the amorphous-to-crystalline transition, experimental results on polycrystalline GeSbTe alloys (GST) films evidenced a Metal-Insulator Transition (MIT) attributed to disorder in the crystalline phase. Here we report on a fundamental advance in the fabrication of GST with out-of-plane stacking of ordered vacancy layers by means of three distinct methods: Molecular Beam Epitaxy, thermal annealing and application of femtosecond laser pulses. We assess the degree of vacancy ordering and explicitly correlate it with the MIT. We further tune the ordering in a controlled fashion attaining a large range of resistivity. Employing ordered GST might allow the realization of cells with larger programming windows.
- 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.
- Item2D layered transport properties from topological insulator Bi2Se3 single crystals and micro flakes(London : Nature Publishing Group, 2016) Chiatti, Olivio; Riha, Christian; Lawrenz, Dominic; Busch, Marco; Dusari, Srujana; Sánchez-Barriga, Jaime; Mogilatenko, Anna; Yashina, Lada V.; Valencia, Sergio; Ünal, Akin A.; Rader, Oliver; Fischer, Saskia F.Low-field magnetotransport measurements of topological insulators such as Bi2Se3 are important for revealing the nature of topological surface states by quantum corrections to the conductivity, such as weak-antilocalization. Recently, a rich variety of high-field magnetotransport properties in the regime of high electron densities (∼1019 cm−3) were reported, which can be related to additional two-dimensional layered conductivity, hampering the identification of the topological surface states. Here, we report that quantum corrections to the electronic conduction are dominated by the surface states for a semiconducting case, which can be analyzed by the Hikami-Larkin-Nagaoka model for two coupled surfaces in the case of strong spin-orbit interaction. However, in the metallic-like case this analysis fails and additional two-dimensional contributions need to be accounted for. Shubnikov-de Haas oscillations and quantized Hall resistance prove as strong indications for the two-dimensional layered metallic behavior. Temperature-dependent magnetotransport properties of high-quality Bi2Se3 single crystalline exfoliated macro and micro flakes are combined with high resolution transmission electron microscopy and energy-dispersive x-ray spectroscopy, confirming the structure and stoichiometry. Angle-resolved photoemission spectroscopy proves a single-Dirac-cone surface state and a well-defined bulk band gap in topological insulating state. Spatially resolved core-level photoelectron microscopy demonstrates the surface stability.
- ItemRevisiting the local structure in Ge-Sb-Te based chalcogenide superlattices(London : Nature Publishing Group, 2016) Casarin, Barbara; Caretta, Antonio; Momand, Jamo; Kooi, Bart J.; Verheijen, Marcel A.; Bragaglia, Valeria; Calarco, Raffaella; Chukalina, Marina; Yu, Xiaoming; Robertson, John; Lange, Felix R.L.; Wuttig, Matthias; Redaelli, Andrea; Varesi, Enrico; Parmigiani, Fulvio; Malvestuto, MarcoThe technological success of phase-change materials in the field of data storage and functional systems stems from their distinctive electronic and structural peculiarities on the nanoscale. Recently, superlattice structures have been demonstrated to dramatically improve the optical and electrical performances of these chalcogenide based phase-change materials. In this perspective, unravelling the atomistic structure that originates the improvements in switching time and switching energy is paramount in order to design nanoscale structures with even enhanced functional properties. This study reveals a high- resolution atomistic insight of the [GeTe/Sb2Te3] interfacial structure by means of Extended X-Ray Absorption Fine Structure spectroscopy and Transmission Electron Microscopy. Based on our results we propose a consistent novel structure for this kind of chalcogenide superlattices.