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We investigate the nanoheteroepitaxy (NHE) of SiGe and Ge quantum dots (QDs) grown on nanotips (NTs) substrates realized in Si(001) wafers. Due to the lattice strain compliance, enabled by the nanometric size of the tip and the limited dot/substrate interface area, which helps to reduce dot/substrate interdiffusion, the strain and SiGe composition in the QDs could be decoupled. This demonstrates a key advantage of the NHE over the Stranski-Krastanow growth mechanism. Nearly semi-spherical, defect-free, ∼100 nm wide SiGe QDs with different Ge contents were successfully grown on the NTs with high selectivity and size uniformity. On the dots, thin dielectric capping layers were deposited, improving the optical properties by the passivation of surface states. Intense photoluminescence was measured from all samples investigated with emission energy, intensity, and spectral linewidth dependent on the SiGe composition of the QDs and the different capping layers. Radiative recombination occurs in the QDs, and its energy matches the results of band-structure calculations that consider strain compliance between the QD and the tip. The NTs arrangement and the selective growth of QDs allow to studying the PL emission from only 3-4 QDs, demonstrating a bright emission and the possibility of selective addressing. These findings will support the design of optoelectronic devices based on CMOS-compatible emitters., (Creative Commons Attribution license.)

Lattice strain in crystals can be exploited to effectively tune their physical properties. In microscopic structures, experimental access to the full strain tensor with spatial resolution at the (sub-)micrometer scale is at the same time very interesting and challenging. In this work, how scanning X-ray diffraction microscopy, an emerging model-free method based on synchrotron radiation, can shed light on the complex, anisotropic deformation landscape within three dimensional (3D) microstructures is shown. This technique allows the reconstruction of all lattice parameters within any type of crystal with submicron spatial resolution and requires no sample preparation. Consequently, the local state of deformation can be fully quantified. Exploiting this capability, all components of the strain tensor in a suspended, strained Ge 1 - x Sn x /Ge microdisk are mapped. Subtle elastic deformations are unambiguously correlated with structural defects, 3D microstructure geometry, and chemical variations, as verified by comparison with complementary electron microscopy and finite element simulations. The methodology described here is applicable to a wide range of fields, from bioengineering to metallurgy and semiconductor research., (© 2024 Wiley‐VCH GmbH.)

A strained Ge quantum well, grown on a SiGe/Si virtual substrate and hosting two electrostatically defined hole spin qubits, is nondestructively investigated by synchrotron-based scanning X-ray diffraction microscopy to determine all its Bravais lattice parameters. This allows rendering the three-dimensional spatial dependence of the six strain tensor components with a lateral resolution of approximately 50 nm. Two different spatial scales governing the strain field fluctuations in proximity of the qubits are observed at <100 nm and >1 μm, respectively. The short-ranged fluctuations have a typical bandwidth of 2 × 10 -4 and can be quantitatively linked to the compressive stressing action of the metal electrodes defining the qubits. By finite element mechanical simulations, it is estimated that this strain fluctuation is increased up to 6 × 10 -4 at cryogenic temperature. The longer-ranged fluctuations are of the 10 -3 order and are associated with misfit dislocations in the plastically relaxed virtual substrate. From this, energy variations of the light and heavy-hole energy maxima of the order of several 100 μeV and 1 meV are calculated for electrodes and dislocations, respectively. These insights over material-related inhomogeneities may feed into further modeling for optimization and design of large-scale quantum processors manufactured using the mainstream Si-based microelectronics technology.

An Al 2 O 3 /ZnO heterojunction was grown on a Si single crystal substrate by subsequent thermal and plasma-assisted atomic layer deposition (ALD) in situ . The band offsets of the heterointerface were then studied by consecutive removal of the layers by argon sputtering, followed by in situ X-ray photoelectron spectroscopy. The valence band maximum and conduction band minimum of Al 2 O 3 are found to be 1.1 eV below and 2.3 eV above those of ZnO, resulting in a type-I staggered heterojunction. An apparent reduction of ZnO to elemental Zn in the interface region was detected in the Zn 2p core level and Zn L 3 MM Auger spectra. This suggests an interface formation different from previous models. The reduction of ZnO to Zn in the interface region accompanied by the creation of oxygen vacancies in ZnO results in an upward band bending at the interface. Therefore, this study suggests that interfacial properties such as the band bending as well as the valence and conduction band offsets should be in situ controllable to a certain extent by careful selection of the process parameters.

InGaN/GaN double heterostructures and multiquantum wells (MQWs) have been successfully developed since more than 20 years for LED lightning applications. Recent developments show that state-of-the-art LEDs benefit from artificially generated V-pit defects. However, the control of structural and chemical properties plays a tremendous role. In this paper, we report on the lateral distribution of V-pit defects and photoluminescence of InGaN/GaN MQWs grown on thick GaN on patterned sapphire substrates. The synchrotron-based scanning X-ray diffraction microscopy technique K-map was employed to locally correlate these properties with the local tilt, strain, and composition of the InGaN/GaN MQW. Compositional fluctuation is the main factor for the variation of photoluminescence intensity and broadening. In turn, V-pit defects align along small-angle grain boundaries and their strain fields are identified as a reason for promoting the InGaN segregation process on a microscale.

We report a detailed advanced materials characterization study on 40 nm thick strained germanium (Ge) layers integrated on 300 mm Si(001) wafers via strain-relaxed silicon-germanium (SiGe) buffer layers. Fast-scanning X-ray microscopy is used to directly image structural inhomogeneities, lattice tilt, thickness, and strain of a functional Ge layer down to the sub-micrometer scale with a real space step size of 750 μm. The structural study shows that the metastable Ge layer, pseudomorphically grown on Si(0.3)Ge(0.7), exhibits an average compressive biaxial strain of -1.27%. By applying a scan area of 100 × 100 μm(2), we observe microfluctuations of strain, lattice tilt, and thickness of ca. ±0.03%, ±0.05°, and ±0.8 nm, respectively. This study confirms the high materials homogeneity of the compressively strained Ge layer realized by the step-graded SiGe buffer approach on 300 mm Si wafers. This presents thus a promising materials science approach for advanced sub-10 nm complementary metal oxide-semiconductor applications based on strain-engineered Ge transistors to outperform current Si channel technologies.

Rare earth praseodymium and cerium oxides have attracted intense research interest in the last few decades, due to their intriguing chemical and physical characteristics. An understanding of the correlation between structure and properties, in particular the surface chemistry, is urgently required for their application in microelectronics, catalysis, optics and other fields. Such an understanding is, however, hampered by the complexity of rare earth oxide materials and experimental methods for their characterisation. Here, we report recent progress in studying high-quality, single crystalline, praseodymium and cerium oxide films as well as ternary alloys grown on Si(111) substrates. Using these well-defined systems and based on a systematic multi-technique surface science approach, the corresponding physical and chemical properties, such as the surface structure, the surface morphology, the bulk-surface interaction and the oxygen storage/release capability, are explored in detail. We show that specifically the crystalline structure and the oxygen stoichiometry of the oxide thin films can be well controlled by the film preparation method. This work leads to a comprehensive understanding of the properties of rare earth oxides and highlights the applications of these versatile materials. Furthermore, methanol adsorption studies are performed on binary and ternary rare earth oxide thin films, demonstrating the feasibility of employing such systems for model catalytic studies. Specifically for ceria systems, we find considerable stability against normal environmental conditions so that they can be considered as a "materials bridge" between surface science models and real catalysts.

Praseodymia films have been exposed to oxygen plasma at room temperature after deposition on Si(111) via molecular beam epitaxy. Different parameters as film thickness, exposure time and flux during plasma treatment have been varied to study their influence on the oxygen plasma oxidation process. The surface near regions have been investigated by means of X-ray photoelectron spectroscopy showing that the plasma treatment transforms the stoichiometry of the films from Pr2O3 to PrO2. Closer inspection of the bulk properties of the films by means of synchrotron radiation based X-ray reflectometry and diffraction confirms this transformation if the films are thicker than some critical thickness of 6 nm. The layer distance of these films is extremely small verifying the completeness of the plasma oxidation process. Thinner films, however, cannot be transformed completely. For all films, less oxidized very thin interlayers are detected by these experimental techniques.

We investigate the structural properties and strain state of Ge nano-structures selectively grown on Si pillars of about 60 nm diameter with different SiGe buffer layers. A matrix of TEOS SiO2 surrounding the Si nano-pillars causes a tensile strain in the top part at the growth temperature of the buffer that reduces the misfit and supports defect-free initial growth. Elastic relaxation plays the dominant role in the further increase of the buffer thickness and subsequent Ge deposition. This method leads to Ge nanostructures on Si that are free from misfit dislocations and other structural defects, which is not the case for direct Ge deposition on these pillar structures. The Ge content of the SiGe buffer is thereby not a critical parameter; it may vary over a relatively wide range.

Advanced semiconductor heterostructures are at the very heart of many modern technologies, including aggressively scaled complementary metal oxide semiconductor transistors for high performance computing and laser diodes for low power solid state lighting applications. The control of structural and compositional homogeneity of these semiconductor heterostructures is the key to success to further develop these state-of-the-art technologies. In this article, we report on the lateral distribution of tilt, composition, and strain across step-graded SiGe strain relaxed buffer layers on 300 mm Si(001) wafers treated with and without chemical-mechanical polishing. By using the advanced synchrotron based scanning X-ray diffraction microscopy technique K-Map together with micro-Raman spectroscopy and Atomic Force Microscopy, we are able to establish a partial correlation between real space morphology and structural properties of the sample resolved at the micrometer scale. In particular, we demonstrate that the lattice plane bending of the commonly observed cross-hatch pattern is caused by dislocations. Our results show a strong local correlation between the strain field and composition distribution, indicating that the adatom surface diffusion during growth is driven by strain field fluctuations induced by the underlying dislocation network. Finally, it is revealed that a superficial chemical-mechanical polishing of cross-hatched surfaces does not lead to any significant change of tilt, composition, and strain variation compared to that of as-grown samples.

In this work the structural and morphological changes of Ce1-xPrxO2-δ (x = 0.20, 0.35 and 0.75) films grown on Si(111) due to post deposition annealing are investigated by low energy electron diffraction combined with a spot profile analysis. The surface of the oxide films exhibit mosaics with large terraces separated by monoatomic steps. It is shown that the Ce/Pr ratio and post deposition annealing temperature can be used to tune the mosaic spread, terrace size and step height of the grains. The morphological changes are accompanied by a phase transition from a fluorite type lattice to a bixbyite structure. Furthermore, at high PDA temperatures a silicate formation via a polycrystalline intermediate state is observed.

Integration of functional oxides on Si substrates could open a pathway to integrate diverse devices on Si-based technology. Oxygen vacancies (Vo(··)) can strongly affect solid state properties of oxides, including the room temperature ferromagnetism (RTFM) in diluted magnetic oxides. Here, we report a systematical study on the RTFM of oxygen vacancy engineered (by Pr(3+) doping) CeO2 epitaxial thin films on Si substrates. High quality, mixed single crystalline Ce1-xPrxO2-δ (x = 0-1) solid solution films were obtained. The Ce ions in CeO2 with a fluorite structure show a Ce(4+)-dominant valence state in all films. The local crystal structures of the films were analyzed in detail. Pr doping creates both Vo(··) and PrO8-complex defects in CeO2 and their relative concentrations vary with the Pr-doping level. The RTFM properties of the films reveal a strong dependence on the relative Vo(··) concentration. The RTFM in the films initially increases with higher Pr-doping levels due to the increase of the F(+) center (Vo(··) with one occupied electron) concentration and completely disappears when x > 0.2, where the magnetic polaron concentration is considered to decline below the percolation threshold, thus long-range FM order can no longer be established. We thus demonstrate the possibility to directly grow RTFM Pr-doped CeO2 films on Si substrates, which can be an interesting candidate for potential magneto-optic or spintronic device applications.

The structural changes of a (111) oriented CeO2 film grown on a Si(111) substrate covered with a hex-Pr2O3(0001) interface layer due to post deposition annealing are investigated. X-ray photoelectron spectroscopy measurements revealing the near surface stoichiometry show that the film reduces continuously upon extended heat treatment. The film is not homogeneously reduced since several coexisting crystalline ceria phases are stabilized due to subsequent annealing at different temperatures as revealed by high resolution low energy electron diffraction and X-ray diffraction. The electron diffraction measurements show that after annealing at 660 °C the ι-phase (Ce7O12) is formed at the surface which exhibits a (√7 × √7)R19.1° structure. Furthermore, a (√27 × √27)R30° surface structure with a stoichiometry close to Ce2O3 is stabilized after annealing at 860 °C which cannot be attributed to any bulk phase of ceria stable at room temperature. In addition, it is shown that the fully reduced ceria (Ce2O3) film exhibits a bixbyite structure. Polycrystalline silicate (CeSi(x)O(y)) and crystalline silicide (CeSi1.67) are formed at 850 °C and detected at the surface after annealing above 900 °C.

The surface morphology of CeO(2)(111) single crystals and silicon supported ceria films is investigated by non-contact atomic force microscopy (NC-AFM) and Kelvin probe force microscopy (KPFM) for various annealing conditions. Annealing bulk samples at 1100 K results in small terraces with rounded ledges and steps with predominantly one O-Ce-O triple layer height while annealing at 1200 K produces well-ordered straight step edges in a hexagonal motif and step bunching. The morphology and topographic details of films are similar, however, films are destroyed upon heating them above 1100 K. KPFM images exhibit uniform terraces on a single crystal surface when the crystal is slowly cooled down, whereas rapid cooling results in a significant inhomogeneity of the surface potential. For films exhibiting large terraces, significant inhomogeneity in the KPFM signal is found even for best possible preparation conditions. Applying X-ray photoelectron spectroscopy (XPS), we find a significant contamination of the bulk ceria sample with fluorine while a possible fluorine contamination of the ceria film is below the XPS detection threshold. Time-of-flight secondary ion mass spectroscopy (TOF-SIMS) reveals an accumulation of fluorine within the first 5 nm below the surface of the bulk sample and a small concentration throughout the crystal.