Epitaxial $ {\rm Ge}_{2} {\rm Sb}_{2} {\rm Te}_{5} $ thin layers were successfully grown in the metastable cubic phase on both slightly lattice‐mismatched (GaSb) and highly lattice‐mismatched (Si) templates. The higher quality of the films grown on (111)‐oriented substrates is attributed to the tendency to form layered structures in the stable bulk phase as well as to the nature of distortion in the metastable cubic phase. (© 2012 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)

The growth by molecular beam epitaxy of GeTe thin films on highly lattice‐mismatched Si(111) substrates is reported. In situ reflection high‐energy electron diffraction and quadrupole mass spectrometry were employed to monitor the growth process in real time and tune the deposition conditions. Epitaxy was achieved in a window of substrate temperatures between 220 and 270 °C, using a Ge/Te flux ratio of ∼0.4. Extensive ex situ X‐ray diffraction characterization showed that the epitaxial layers crystallize in the rhombohedrally distorted rocksalt structure α‐GeTe, with orientation relationships to the substrate α‐GeTe[0001] ‖ Si[111] and α‐GeTe〈10${\bar {1}}$0〉 ‖ Si〈$11{\bar {2}}$〉. ω‐scans of the α‐GeTe(000n) reflections (n = 3, 6, 9) exhibit a full width at half maximum between 10 and 20 arcsec, indicating small mosaicity. However, a large twist is observed (∼14°), pointing to the presence of rotational domains. In addition, the layer matrix is affected by twinning. The epitaxial films exhibit a slight tensile in‐plane strain, which might be due to the difference in thermal expansion coefficients between α‐GeTe and Si, and/or small deviation from stoichiometric composition, i.e., vacancies in the Ge sub‐lattice.

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A combined structure and stoichiometry study on the growth behavior of single crystalline Ge(111) layers on PrO2(111)∕Si(111) heterostructures is presented. Ex situ x-ray diffraction techniques indicate that the interaction between Ge and PrO2(111) results in a complete reduction of the buffer oxide to a cubic Pr2O3(111) film structure. In situ reflection high energy electron diffraction, x-ray and ultraviolet photoelectron spectroscopy studies demonstrate that this chemical reduction of the oxide support occurs during the initial Ge growth stage. The interaction of PrO2 with Ge results in the formation of an amorphous Ge oxide layer by the diffusion of lattice oxygen from the dielectric to the forming semiconductor deposit. After the complete conversion of PrO2 to cubic Pr2O3, the supply of reactive lattice oxygen is exhausted and the continuous Ge deposition reduces the initially formed amorphous GeO2-like film to GeO. The sublimation of volatile GeO uncovers the single crystalline cubic Pr2O3(111) film surface which provides a thermodynamically stable template for elemental Ge heteroepitaxy. A Volmer–Weber growth mode is observed which results after island coalescence in the formation of atomically smooth, single crystalline Ge(111) layers.

Coherent phonons (CPs) generated by laser pulses on the femtosecond scale have been proposed as a means to achieve ultrafast, nonthermal switching in phase-change materials such as Ge 2 Sb 2 Te 5 (GST). Here we use ultrafast optical pump pulses to induce coherent acoustic phonons and stroboscopically measure the corresponding lattice distortions in GST using 100-ps x-ray pulses from the European Synchrotron Radiation Facility (ESRF) storage ring. A linear-chain model provides a good description of the observed changes in the diffraction signal; however, the magnitudes of the measured shifts are too large to be explained by thermal effects alone, implying the presence of excited-state effects in addition to temperature-driven expansion. The information on the movement of atoms during the excitation process can lead to greater insight into the possibilities of using CP-induced phase transitions in GST.

Engineered wafer systems are an important materials science approach to achieve the global integration of single crystalline Ge layers on the Si platform. Here, we report the formation of single crystalline, fully relaxed Ge(111) films by molecular beam epitaxial overgrowth of cubic Pr oxide buffers on Si(111) substrates. Reflection high-energy electron diffraction, scanning electron microscopy, and x-ray reflectivity show that the Ge epilayer is closed, flat, and has a sharp interface with the underlying oxide template. Synchrotron radiation grazing incidence x-ray diffraction and transmission electron microscopy reveal the type-A/B/A epitaxial relationship of the Ge(111)/cubic Pr2O3(111)/Si(111) heterostructure, a result also corroborated by theoretical ab initio structure calculations. Secondary ion mass spectroscopy confirms the absence of Pr and Si impurities in the Ge(111) epilayer, even after an annealing at 825 °C.

The defect structure of Ge(111) epilayers grown by molecular beam epitaxy on cubic Pr2O3(111)/Si(111) support systems was investigated by means of transmission electron microscopy and laboratory-based x-ray diffraction techniques. Three main types of defects were identified, namely, rotation twins, microtwins, and stacking faults, and studied as a function of Ge film thickness and after annealing at 825 °C in ultrahigh vacuum. Rotation twins were found to be localized at the Ge(111)/cubic Pr2O3(111) interface and their amount could be lowered by the thermal treatment. Microtwins across {111¯} were detected only in closed Ge films, after Ge island coalescence. The fraction of Ge film volume affected by microtwinning is constant within the thickness range of ∼20–260 nm. Beyond 260 nm, the density of microtwins is clearly reduced, resulting in thick layers with a top part of higher crystalline quality. Microtwins resulted insensitive to the postdeposition annealing. Instead, the density of stacking faults across {111¯} planes decreases with the thermal treatment. In conclusion, the defect density was proved to diminish with increasing Ge thickness and after annealing. Moreover, it is noteworthy that the annealing generates a tetragonal distortion in the Ge films, which get in-plane tensely strained, probably due to thermal mismatch between Ge and Si.

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