Jos E. Boschker

Interface formation of two- and three-dimensionally bonded materials in the case of GeTe–Sb2Te3 superlattices

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.

Surface Reconstruction-Induced Coincidence Lattice Formation Between Two-Dimensionally Bonded Materials and a Three-Dimensionally Bonded Substrate

Sb2Te3 films are used for studying the epitaxial registry between two-dimensionally bonded (2D) materials and three-dimensional bonded (3D) substrates. In contrast to the growth of 3D materials, it is found that the formation of coincidence lattices between Sb2Te3 and Si(111) depends on the geometry and dangling bonds of the reconstructed substrate surface. Furthermore, we show that the epitaxial registry can be influenced by controlling the Si(111) surface reconstruction and confirm the results for ultrathin films.

Giant Rashba‐Type Spin Splitting in Ferroelectric GeTe(111)

Photoelectron spectroscopy in combination with piezoforce microscopy reveals that the helicity of Rashba bands is coupled to the nonvolatile ferroelectric polarization of GeTe(111). A novel surface Rashba band is found and fingerprints of a bulk Rashba band are identified by comparison with density functional theory calculations.

Metal - Insulator Transition Driven by Vacancy Ordering in GeSbTe Phase Change Materials

Phase 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.

Far-Infrared and Raman Spectroscopy Investigation of Phonon Modes in Amorphous and Crystalline Epitaxial GeTe-Sb2Te3 Alloys.

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.

Crossover from Spin-Flop Coupling to Collinear Spin Alignment in Antiferromagnetic/Ferromagnetic Nanostructures

The technologically important exchange coupling in antiferromagnetic/ferromagnetic bilayers is investigated for embedded nanostructures defined in a LaFeO(3)/La(0.7)Sr(0.3)MnO(3) bilayer. Exploiting the element specificity of soft X-ray spectromicroscopy, we selectively probe the magnetic order in the two layers. A transition from perpendicular to parallel spin alignment is observed for these nanostructures, dependent on size and crystalline orientation. The results show that shape-induced anisotropy in the antiferromagnet can override the interface exchange coupling in spin-flop coupled nanostructures.

Structural phases driven by oxygen vacancies at the La0.7Sr0.3MnO3/SrTiO3 hetero-interface

An oxygen vacancy driven structural response at the epitaxial interface between La0.7Sr0.3MnO3 films and SrTiO3 substrates is reported. A combined scanning transmission electron microscopy and electron energy loss spectroscopy study reveal the presence of an elongated out-of-plane lattice parameter, coupled to oxygen vacancies and reduced manganese oxidation state at the La0.7Sr0.3MnO3 side of the interface. Density functional theory calculations support that the measured interface structure is a disordered oxygen deficient brownmillerite structure. The effect of oxygen vacancy mobility is assessed, revealing an ordering of the vacancies with time.

Electrical performance of phase change memory cells with Ge3Sb2Te6 deposited by molecular beam epitaxy

Here, we report on the electrical characterization of phase change memory cells containing a Ge3Sb2Te6 (GST) alloy grown in its crystalline form by Molecular Beam Epitaxy (MBE). It is found that the high temperature growth on the amorphous substrate results in a polycrystalline film exhibiting a rough surface with a grain size of approximately 80–150 nm. A detailed electrical characterization has been performed, including I-V characteristic curves, programming curves, set operation performance, crystallization activation at low temperature, and resistance drift, in order to determine the material related parameters. The results indicate very good alignment of the electrical parameters with the current state-of-the-art GST, deposited by physical vapor deposition. Such alignment enables a possible employment of the MBE deposition technique for chalcogenide materials in the phase change memory technology, thus leading to future studies of as-deposited crystalline chalcogenides as integrated in electrical veh...

Surface stability of epitaxial La0.7Sr0.3MnO3 thin films on (111)-oriented SrTiO3

We report on the stability of the La0.7Sr0.3MnO3 thin film surface when deposited on (111)-oriented SrTiO3. For ultrathin La0.7Sr0.3MnO3 films, an initial 3-dimensional morphology is observed, which becomes 2-dimensional with increasing film thickness. For even thicker samples, we show that the surface morphology evolves from 2-dimensional to 3-dimensional and that this observation is consistent with an Asaro-Tiller-Grinfeld instability, which can be controlled by the deposition temperature. This allows for synthesis of films with step-and-terrace surfaces over a wide range of thicknesses. Structural characterization by x-ray diffraction and transmission electron microscopy shows that the films are strained to the SrTiO3 substrate and reveals the presence of an elongated out-of-plane lattice parameter at the interface with SrTiO3.

Qualitative determination of surface roughness by in situ reflection high energy electron diffraction

We demonstrate that a qualitative measure of the surface roughness can be obtained by using in situ reflection high energy electron diffraction. The in situ measurements of the surface roughness are found to be in agreement with the topography, as determined by ex situ atomic force microscopy. Relying on this method, we study the surface roughening during pulsed laser deposition of La0.7Sr0.3MnO3 and investigate the quality of (001)-oriented SrTiO3 substrates with a TiO2 termination.