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- 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.
- 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.
- ItemUnderstanding the growth mechanism of graphene on Ge/Si(001) surfaces(London : Nature Publishing Group, 2016) Dabrowski, J.; Lippert, G.; Avila, J.; Baringhaus, J.; Colambo, I.; Dedkov, Yu S.; Herziger, F.; Lupina, G.; Maultzsch, J.; Schaffus, T.; Schroeder, T.; Kot, M.; Tegenkamp, C.; Vignaud, D.; Asensio, M.-C.The practical difficulties to use graphene in microelectronics and optoelectronics is that the available methods to grow graphene are not easily integrated in the mainstream technologies. A growth method that could overcome at least some of these problems is chemical vapour deposition (CVD) of graphene directly on semiconducting (Si or Ge) substrates. Here we report on the comparison of the CVD and molecular beam epitaxy (MBE) growth of graphene on the technologically relevant Ge(001)/Si(001) substrate from ethene (C2H4) precursor and describe the physical properties of the films as well as we discuss the surface reaction and diffusion processes that may be responsible for the observed behavior. Using nano angle resolved photoemission (nanoARPES) complemented by transport studies and Raman spectroscopy as well as density functional theory (DFT) calculations, we report the direct observation of massless Dirac particles in monolayer graphene, providing a comprehensive mapping of their low-hole doped Dirac electron bands. The micrometric graphene flakes are oriented along two predominant directions rotated by 30° with respect to each other. The growth mode is attributed to the mechanism when small graphene “molecules” nucleate on the Ge(001) surface and it is found that hydrogen plays a significant role in this process.
- 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.
- 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.
- 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.
- ItemAtomically precise semiconductor-graphene and hBN interfaces by Ge intercalation(London : Nature Publishing Group, 2015) Verbitskiy, N.I.; Fedorov, A.V.; Profeta, G.; Stroppa, A.; Petaccia, L.; Senkovskiy, B.; Nefedov, A.; Wöll, C.; Usachov, D.Yu.; Vyalikh, D.V.; Yashina, L.V.; Eliseev, A.A.; Pichler, T.; Grüneis, A.The full exploration of the potential, which graphene offers to nanoelectronics requires its integration into semiconductor technology. So far the real-world applications are limited by the ability to concomitantly achieve large single-crystalline domains on dielectrics and semiconductors and to tailor the interfaces between them. Here we show a new direct bottom-up method for the fabrication of high-quality atomically precise interfaces between 2D materials, like graphene and hexagonal boron nitride (hBN), and classical semiconductor via Ge intercalation. Using angle-resolved photoemission spectroscopy and complementary DFT modelling we observed for the first time that epitaxially grown graphene with the Ge monolayer underneath demonstrates Dirac Fermions unaffected by the substrate as well as an unperturbed electronic band structure of hBN. This approach provides the intrinsic relativistic 2D electron gas towards integration in semiconductor technology. Hence, these new interfaces are a promising path for the integration of graphene and hBN into state-of-the-art semiconductor technology.
- ItemInterface control by homoepitaxial growth in pulsed laser deposited iron chalcogenide thin films(London : Nature Publishing Group, 2015) Molatta, Sebastian; Haindl, Silvia; Trommler, Sascha; Schulze, Michael; Wurmehl, Sabine; Hühne, RubenThin film growth of iron chalcogenides by pulsed laser deposition (PLD) is still a delicate issue in terms of simultaneous control of stoichiometry, texture, substrate/film interface properties, and superconducting properties. The high volatility of the constituents sharply limits optimal deposition temperatures to a narrow window and mainly challenges reproducibility for vacuum based methods. In this work we demonstrate the beneficial introduction of a semiconducting FeSe1−xTex seed layer for subsequent homoepitaxial growth of superconducting FeSe1−xTex thin film on MgO substrates. MgO is one of the most favorable substrates used in superconducting thin film applications, but the controlled growth of iron chalcogenide thin films on MgO has not yet been optimized and is the least understood. The large mismatch between the lattice constants of MgO and FeSe1−xTex of about 11% results in thin films with a mixed texture, that prevents further accurate investigations of a correlation between structural and electrical properties of FeSe1−xTex. Here we present an effective way to significantly improve epitaxial growth of superconducting FeSe1−xTex thin films with reproducible high critical temperatures (≥17 K) at reduced deposition temperatures (200 °C–320 °C) on MgO using PLD. This offers a broad scope of various applications.
- 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.
- ItemIntrinsic and extrinsic pinning in NdFeAs(O,F): Vortex trapping and lock-in by the layered structure(London : Nature Publishing Group, 2016) Tarantini, C.; Iida, K.; Hänisch, J.; Kurth, F.; Jaroszynski, J.; Sumiya, N.; Chihara, M.; Hatano, T.; Ikuta, H.; Schmidt, S.; Seidel, P.; Holzapfel, B.; Larbalestier, D.C.Fe-based superconductors (FBS) present a large variety of compounds whose properties are affected to different extents by their crystal structures. Amongst them, the REFeAs(O,F) (RE1111, RE being a rare-earth element) is the family with the highest critical temperature Tc but also with a large anisotropy and Josephson vortices as demonstrated in the flux-flow regime in Sm1111 (Tc ∼ 55 K). Here we focus on the pinning properties of the lower-Tc Nd1111 in the flux-creep regime. We demonstrate that for H//c critical current density Jc at high temperatures is dominated by point-defect pinning centres, whereas at low temperatures surface pinning by planar defects parallel to the c-axis and vortex shearing prevail. When the field approaches the ab-planes, two different regimes are observed at low temperatures as a consequence of the transition between 3D Abrikosov and 2D Josephson vortices: one is determined by the formation of a vortex-staircase structure and one by lock-in of vortices parallel to the layers. This is the first study on FBS showing this behaviour in the full temperature, field, and angular range and demonstrating that, despite the lower Tc and anisotropy of Nd1111 with respect to Sm1111, this compound is substantially affected by intrinsic pinning generating a strong ab-peak in Jc.