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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.
- ItemGrowth of crystalline phase change materials by physical deposition methods(Abingdon : Taylor & Francis Group, 2017) Boschker, Jos E.; Calarco, RaffaellaPhase change materials are a technologically important materials class and are used for data storage in rewritable DVDs and in phase change random access memory. Furthermore, new applications for phase change materials are emerging. Phase change materials with a high structural quality, such as offered by epitaxial films, are needed in order to study the fundamental properties of phase change materials and to improve our understanding of this materials class. Here, we review the progress made in the growth of crystalline phase change materials by physical methods, such as molecular beam epitaxy, sputtering, and pulsed laser deposition. First, we discuss the difference and similarities between these physical deposition methods and the crystal structures of Ge2Sb2Te5, the prototype phase change material. Next, we focus on the growth of epitiaxial GST films on (0 0 1)- and (1 1 1)-oriented substrates, leading to the conclusion that (1 1 1)-oriented substrates are preferred for the growth of phase change materials. Finally, the growth of GeTe/Sb2Te3 superlattices on amorphous and single crystalline substrates is discussed.
- 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.
- ItemFerroelectric Control of the Spin Texture in GeTe(Washington, DC : ACS Publ., 2018-1-30) Rinaldi, Christian; Varotto, Sara; Asa, Marco; Sławińska, Jagoda; Fujii, Jun; Vinai, Giovanni; Cecchi, Stefano; Di Sante, Domenico; Calarco, Raffaella; Vobornik, Ivana; Panaccione, Giancarlo; Picozzi, Silvia; Bertacco, RiccardoThe electric and nonvolatile control of the spin texture in semiconductors would represent a fundamental step toward novel electronic devices combining memory and computing functionalities. Recently, GeTe has been theoretically proposed as the father compound of a new class of materials, namely ferroelectric Rashba semiconductors. They display bulk bands with giant Rashba-like splitting due to the inversion symmetry breaking arising from the ferroelectric polarization, thus allowing for the ferroelectric control of the spin. Here, we provide the experimental demonstration of the correlation between ferroelectricity and spin texture. A surface-engineering strategy is used to set two opposite predefined uniform ferroelectric polarizations, inward and outward, as monitored by piezoresponse force microscopy. Spin and angular resolved photoemission experiments show that these GeTe(111) surfaces display opposite sense of circulation of spin in bulk Rashba bands. Furthermore, we demonstrate the crafting of nonvolatile ferroelectric patterns in GeTe films at the nanoscale by using the conductive tip of an atomic force microscope. Based on the intimate link between ferroelectric polarization and spin in GeTe, ferroelectric patterning paves the way to the investigation of devices with engineered spin configurations.
- ItemEvolution of Low-Frequency Vibrational Modes in Ultrathin GeSbTe Films(Weinheim : Wiley-VCH, 2021) Zallo, Eugenio; Dragoni, Daniele; Zaytseva, Yuliya; Cecchi, Stefano; Borgardt, Nikolai I.; Bernasconi, Marco; Calarco, RaffaellaGeSbTe (GST) phase-change alloys feature layered crystalline structures made of lamellae separated by van der Waals (vdW) gaps. This work sheds light on the dependence of interlamellae interactions at the vdW gap on film thickness of GST alloys as probed by vibrational spectroscopy. Molecular beam epitaxy is used for designing GST layers down to a single lamella. By combining density-functional theory and Raman spectroscopy, a direct and simple method is demonstrated to identify the thickness of the GST film. The shift of the vibrational modes is studied as a function of the layer size, and the low-frequency range opens up a new route to probe the number of lamellae for different GST compositions. Comparison between experimental and theoretical Raman spectra highlights the precision growth control obtained by the epitaxial technique.
- 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.
- ItemElectrical and optical properties of epitaxial binary and ternary GeTe-Sb2Te3 alloys(London : Nature Publishing, 2018) Boschker, Jos E.; Lü, Xiang; Bragaglia, Valeria; Wang,Ruining; Grahn, Holger T.; Calarco, RaffaellaPhase change materials such as pseudobinary GeTe-Sb2Te3 (GST) alloys are an essential part of existing and emerging technologies. Here, we investigate the electrical and optical properties of epitaxial phase change materials: α-GeTe, Ge2Sb2Te5 (GST225), and Sb2Te3. Temperature-dependent Hall measurements reveal a reduction of the hole concentration with increasing temperature in Sb2Te3 that is attributed to lattice expansion, resulting in a non-linear increase of the resistivity that is also observed in GST225. Fourier transform infrared spectroscopy at room temperature demonstrates the presence of electronic states within the energy gap for α-GeTe and GST225. We conclude that these electronic states are due to vacancy clusters inside these two materials. The obtained results shed new light on the fundamental properties of phase change materials such as the high dielectric constant and persistent photoconductivity and have the potential to be included in device simulations.
- ItemSub-nanometre resolution of atomic motion during electronic excitation in phase-change materials(London : Nature Publishing, 2016) Mitrofanov, Kirill V.; Fons, Paul; Makino, Kotaro; Terashima, Ryo; Shimada, Toru; Kolobov, Alexander, V.; Tominaga, Junji; Bragaglia, Valeria; Giussani, Alessandro; Calarco, Raffaella; Riechert, Henning; Sato, Takahiro; Katayama, Tetsuo; Ogawa, Kanade; Togashi, Tadashi; Yabashi, Makina; Wall, Simon; Brewe, Dale; Hase, MuneakiPhase-change materials based on Ge-Sb-Te alloys are widely used in industrial applications such as nonvolatile memories, but reaction pathways for crystalline-to-amorphous phase-change on picosecond timescales remain unknown. Femtosecond laser excitation and an ultrashort x-ray probe is used to show the temporal separation of electronic and thermal effects in a long-lived (>100 ps) transient metastable state of Ge2Sb2Te5 with muted interatomic interaction induced by a weakening of resonant bonding. Due to a specific electronic state, the lattice undergoes a reversible nondestructive modification over a nanoscale region, remaining cold for 4 ps. An independent time-resolved x-ray absorption fine structure experiment confirms the existence of an intermediate state with disordered bonds. This newly unveiled effect allows the utilization of non-thermal ultra-fast pathways enabling artificial manipulation of the switching process, ultimately leading to a redefined speed limit and improved energy efficiency and reliability of phase-change memory technologies.