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- ItemThermal annealing studies of GeTe-Sb2Te3 alloys with multiple interfaces(New York : American Institute of Physics, 2017) Bragaglia, Valeria; Mio, Antonio M.; Calarco, RaffaellaA high degree of vacancy ordering is obtained by annealing amorphous GeTe-Sb2Te3 (GST) alloys deposited on a crystalline substrate, which acts as a template for the crystallization. Under annealing the material evolves from amorphous to disordered rocksalt, to ordered rocksalt with vacancies arranged into (111) oriented layers, and finally converts into the stable trigonal phase. The role of the interface in respect to the formation of an ordered crystalline phase is studied by comparing the transformation stages of crystalline GST with and without a capping layer. The capping layer offers another crystallization interface, which harms the overall crystalline quality.
- ItemTextured Sb2Te3 films and GeTe/Sb2Te3 superlattices grown on amorphous substrates by molecular beam epitaxy(New York : American Institute of Physics, 2017) Boschker, Jos E.; Tisbi, E.; Placidi, E.; Momand, Jamo; Redaelli, Andrea; Kooi, Bart J.; Arciprete, Fabrizio; Calarco, RaffaellaThe realization of textured films of 2-dimensionally (2D) bonded materials on amorphous substrates is important for the integration of this material class with silicon based technology. Here, we demonstrate the successful growth by molecular beam epitaxy of textured Sb2Te3 films and GeTe/Sb2Te3 superlattices on two types of amorphous substrates: carbon and SiO2. X-ray diffraction measurements reveal that the out-of-plane alignment of grains in the layers has a mosaic spread with a full width half maximum of 2.8°. We show that a good texture on SiO2 is only obtained for an appropriate surface preparation, which can be performed by ex situ exposure to Ar+ ions or by in situ exposure to an electron beam. X-ray photoelectron spectroscopy reveals that this surface preparation procedure results in reduced oxygen content. Finally, it is observed that film delamination can occur when a capping layer is deposited on top of a superlattice with a good texture. This is attributed to the stress in the capping layer and can be prevented by using optimized deposition conditions of the capping layer. The obtained results are also relevant to the growth of other 2D materials on amorphous substrates.
- ItemImproved structural and electrical properties in native Sb2Te3/GexSb2Te3+x van der Waals superlattices due to intermixing mitigation(New York : American Institute of Physics, 2017) Cecchi, Stefano; Zallo, Eugenio; Momand, Jamo; Wang, Ruining; Kooi, Bart J.; Verheijen, Marcel A.; Calarco, RaffaellaSuperlattices made of Sb2Te3/GeTe phase change materials have demonstrated outstanding performance with respect to GeSbTe alloys in memory applications. Recently, epitaxial Sb2Te3/GeTe superlattices were found to feature GexSb2Te3+x blocks as a result of intermixing between constituting layers. Here we present the epitaxy and characterization of Sb2Te3/GexSb2Te3+x van der Waals superlattices, where GexSb2Te3+x was intentionally fabricated. X-ray diffraction, Raman spectroscopy, scanning transmission electron microscopy, and lateral electrical transport data are reported. The intrinsic 2D nature of both sublayers is found to mitigate the intermixing in the structures, significantly improving the interface sharpness and ultimately the superlattice structural and electrical properties.
- ItemFormation of resonant bonding during growth of ultrathin GeTe films(London : Nature Publishing Group, 2017) Wang, Ruining; Zhang, Wei; Momand, Jamo; Ronneberger, Ider; Boschker, Jos E.; Mazzarello, Riccardo; Kooi, Bart J.; Riechert, Henning; Wuttig, Matthias; Calarco, RaffaellaA highly unconventional growth scenario is reported upon deposition of GeTe films on the hydrogen passivated Si(111) surface. Initially, an amorphous film forms for growth parameters that should yield a crystalline material. The entire amorphous film then crystallizes once a critical thickness of four GeTe bilayers is reached, subsequently following the GeTe(111)
- 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.
- ItemModulation of van der Waals and classical epitaxy induced by strain at the Si step edges in GeSbTe alloys(London : Nature Publishing Group, 2017) Zallo, Eugenio; Cecchi, Stefano; Boschker, Jos E.; Mio, Antonio M.; Arciprete, Fabrizio; Privitera, Stefania; Calarco, RaffaellaThe present work displays a route to design strain gradients at the interface between substrate and van der Waals bonded materials. The latter are expected to grow decoupled from the substrates and fully relaxed and thus, by definition, incompatible with conventional strain engineering. By the usage of passivated vicinal surfaces we are able to insert strain at step edges of layered chalcogenides, as demonstrated by the tilt of the epilayer in the growth direction with respect of the substrate orientation. The interplay between classical and van der Waals epitaxy can be modulated with an accurate choice of the substrate miscut. High quality crystalline GexSb2Te3+x with almost Ge1Sb2Te4 composition and improved degree of ordering of the vacancy layers is thus obtained by epitaxial growth of layers on 3–4° stepped Si substrates. These results highlight that it is possible to build and control strain in van der Waals systems, therefore opening up new prospects for the functionalization of epilayers by directly employing vicinal substrates.
- 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.
- 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.
- ItemCoincident-site lattice matching during van der Waals epitaxy(London : Nature Publishing Group, 2015) Boschker, Jos E.; Galves, Lauren A.; Flissikowski, Timur; Lopes, Joao Marcelo J.; Kiemer, Alexandra K.; Riechert, Henning; Calarco, RaffaellaVan der Waals (vdW) epitaxy is an attractive method for the fabrication of vdW heterostructures. Here Sb2Te3 films grown on three different kind of graphene substrates (monolayer epitaxial graphene, quasi freestanding bilayer graphene and the SiC (6√3 × 6√3)R30° buffer layer) are used to study the vdW epitaxy between two 2-dimensionally (2D) bonded materials. It is shown that the Sb2Te3 /graphene interface is stable and that coincidence lattices are formed between the epilayers and substrate that depend on the size of the surface unit cell. This demonstrates that there is a significant, although relatively weak, interfacial interaction between the two materials. Lattice matching is thus relevant for vdW epitaxy with two 2D bonded materials and a fundamental design parameter for vdW heterostructures.