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- 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.
- 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.
- ItemInterface formation of two- and three-dimensionally bonded materials in the case of GeTe–Sb2Te3 superlattices(Cambridge : Royal Society of Chemistry, 2015) Momand, Jamo; Wang, Ruining; Boschker, Jos E.; Verheijen, Marcel A.; Calarcob, Raffaella; Kooi, Bart J.GeTe–Sb2Te3 superlattices are nanostructured phase-change materials which are under intense investigation for non-volatile memory applications. They show superior properties compared to their bulk counterparts and significant efforts exist to explain the atomistic nature of their functionality. The present work sheds new light on the interface formation between GeTe and Sb2Te3, contradicting previously proposed models in the literature. For this purpose [GeTe(1 nm)–Sb2Te3(3 nm)]15 superlattices were grown on passivated Si(111) at 230 °C using molecular beam epitaxy and they have been characterized particularly with cross-sectional HAADF scanning transmission electron microscopy. Contrary to the previously proposed models, it is found that the ground state of the film actually consists of van der Waals bonded layers (i.e. a van der Waals heterostructure) of Sb2Te3 and rhombohedral GeSbTe. Moreover, it is shown by annealing the film at 400 °C, which reconfigures the superlattice into bulk rhombohedral GeSbTe, that this van der Waals layer is thermodynamically favored. These results are explained in terms of the bonding dimensionality of GeTe and Sb2Te3 and the strong tendency of these materials to intermix. The findings debate the previously proposed switching mechanisms of superlattice phase-change materials and give new insights in their possible memory application.
- 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) 
- 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.