Tobias U. Schülli

Imaging of strain and lattice orientation by quick scanning X-ray microscopy combined with three-dimensional reciprocal space mapping

Numerous imaging methods have been developed over recent years in order to study materials at the nanoscale. Within this context, scanning X-ray diffraction microscopy has become a routine technique, giving access to structural properties with sub-micrometre resolution. This article presents an optimized technique and an associated software package which have been implemented at the ID01 beamline (ESRF, Grenoble). A structural scanning probe microscope with intriguing imaging qualities is obtained. The technique consists in a two-dimensional quick continuous mapping with sub-micrometre resolution of a sample at a given reciprocal space position. These real space maps are made by continuously moving the sample while recording scattering images with a fast two-dimensional detector for every point along a rocking curve. Five-dimensional data sets are then produced, consisting of millions of detector images. The images are processed by the user-friendly X-ray strain orientation calculation software (XSOCS), which has been developed at ID01 for automatic analysis. It separates tilt and strain and generates two-dimensional maps of these parameters. At spatial resolutions of typically 200–800 nm, this quick imaging technique achieves strain sensitivity below Δa/a = 10−5 and a resolution of tilt variations down to 10−3° over a field of view of 100 × 100 µm.

Intergrowth structure and aluminium zoning of a zeolite ZSM-5 crystal as resolved by synchrotron-based micro-X-ray diffraction imaging

Zeolites represent an important group of heterogeneous catalysts and are heavily used in the petrochemical and refining industries.[1] Since their discovery, zeolites with MFI topology, namely ZSM-5, have been utilized in a number of large-scale industrial applications. The unique combination of acidic properties and pore architecture[2] enabled their use as solid acid catalysts in the alkylation of arenes,[3] the oligomerization of light olefins,[4] and the methanol-to-hydrocarbon reaction.[5] The internal crystallographic architecture, microand mesoporosity, as well as the 3D distribution of Bronsted acid sites play a crucial role in the catalytic performance of zeolites.

X-ray diffraction from rectangular slits

It is shown that for micrometre-sized beams the X-ray diffraction from slits is a source of strong parasitic background, even for slits of high quality. In order to illustrate this effect, the coherent diffraction from rectangular slits has been studied in detail. A large number of interference fringes with strong visibility have been observed using a single set of slits made of polished cylinders. For very small apertures, asymmetrical slits generate asymmetrical patterns. This pattern is calculated from the theory of electromagnetic field propagation and compared with experiment in the far-field regime. The use of guard slits to remove Fraunhofer diffraction from the beam-defining slits is treated theoretically. Numerical simulations yield the optimum aperture of the guard slits with respect to the distance to the primary slits. Diffraction theory is shown to be essential to understand how to reduce the background-to-signal ratio in high-resolution experiments.

Anomalous x-ray diffraction on InAs/GaAs quantum dot systems

Free-standing InAs quantum dots on a GaAs (001) substrate have been investigated using grazing incidence x-ray diffraction. To suppress the strong scattering contribution from the GaAs substrate, we performed anomalous diffraction experiments at the superstructure (200) reflection, showing that the relative intensities from the dots and the substrate undergo a significant change with the x-ray energy below and above the As K edge. Since the signal from the substrate material can essentially be suppressed, this method is ideally suited for the investigation of strain, shape, and interdiffusion of buried quantum dots and quantum dots embedded in heteroepitaxial multilayers. In addition, we show that it can be used as a tool for studying wetting layers.

Correlation of electrical and structural properties of single as-grown GaAs nanowires on Si (111) substrates.

We present the results of the study of the correlation between the electrical and structural properties of individual GaAs nanowires measured in their as-grown geometry. The resistance and the effective charge carrier mobility were extracted for several nanowires, and subsequently, the same nano-objects were investigated using X-ray nanodiffraction. This revealed a number of perfectly stacked zincblende and twinned zincblende units separated by axial interfaces. Our results suggest a correlation between the electrical parameters and the number of intrinsic interfaces.

Strain and lattice orientation distribution in SiN/Ge complementary metal–oxide–semiconductor compatible light emitting microstructures by quick x-ray nano-diffraction microscopy

This paper presents a study of the spatial distribution of strain and lattice orientation in CMOS-fabricated strained Ge microstripes using high resolution x-ray micro-diffraction. The recently developed model-free characterization tool, based on a quick scanning x-ray diffraction microscopy technique can image strain down to levels of 10−5 (Δa/a) with a spatial resolution of ∼0.5 μm. Strain and lattice tilt are extracted using the strain and orientation calculation software package X-SOCS. The obtained results are compared with the biaxial strain distribution obtained by lattice parameter-sensitive μ-Raman and μ-photoluminescence measurements. The experimental data are interpreted with the help of finite element modeling of the strain relaxation dynamics in the investigated structures.

Inversion Domain Boundaries in GaN Wires Revealed by Coherent Bragg Imaging

Interfaces between polarity domains in nitride semiconductors, the so-called Inversion Domain Boundaries (IDB), have been widely described, both theoretically and experimentally, as perfect interfaces (without dislocations and vacancies). Although ideal planar IDBs are well documented, the understanding of their configurations and interactions inside crystals relies on perfect-interface assumptions. Here, we report on the microscopic configuration of IDBs inside n-doped gallium nitride wires revealed by coherent X-ray Bragg imaging. Complex IDB configurations are evidenced with 6 nm resolution and the absolute polarity of each domain is unambiguously identified. Picoscale displacements along and across the wire are directly extracted from several Bragg reflections using phase retrieval algorithms, revealing rigid relative displacements of the domains and the absence of microscopic strain away from the IDBs. More generally, this method offers an accurate inner view of the displacements and strain of interacting defects inside small crystals that may alter optoelectronic properties of semiconductor devices.

Compliant substrate versus plastic relaxation effects in Ge nanoheteroepitaxy on free-standing Si(001) nanopillars

We report on the structural characterization of Ge clusters selectively grown by chemical vapor deposition on free-standing 50 nm wide Si(001) nanopillars. Synchrotron based x-ray diffraction studies and transmission electron microscopy were performed to experimentally verify the nanoheteroepitaxy theory as a technique to grow high quality Ge on Si(001). Although the structure dimensions are comparable to the theoretical values required for the strain partitioning phenomenon, the compliant character of Si is not unambiguously proven. In consequence, the strain is relieved by nucleation of misfit dislocations at the Ge/Si interface. By gliding out of threading arms, high quality Ge nanostructures are achieved.

In situ investigation of the island nucleation of Ge on Si(001) using x-ray scattering methods

The growth of Ge on Si(001) is investigated in situ at 500 and 600°C, combining grazing incidence diffraction, multiple wavelength anomalous diffraction, and small angle scattering. This allows probing simultaneously the island shape, strain state, composition, and the transition from wetting layer to island growth. At 500°C no intermixing occurs. The wetting layer is found to decrease by one atomic layer at the onset of island nucleation. At 600°C interdiffusion plays an important role in strain relaxation leading to a more stable wetting layer. Small angle scattering yields the island morphology and shows the transition from pyramids to multifacetted domes.

Growth and relaxation processes in Ge nanocrystals on free-standing Si(001) nanopillars.

We study the growth and relaxation processes of Ge crystals selectively grown by chemical vapour deposition on free-standing 90 nm wide Si(001) nanopillars. Epi-Ge with thickness ranging from 4 to 80 nm was characterized by synchrotron based x-ray diffraction and transmission electron microscopy. We found that the strain in Ge nanostructures is plastically released by nucleation of misfit dislocations, leading to degrees of relaxation ranging from 50 to 100%. The growth of Ge nanocrystals follows the equilibrium crystal shape terminated by low surface energy (001) and {113} facets. Although the volumes of Ge nanocrystals are homogeneous, their shape is not uniform and the crystal quality is limited by volume defects on {111} planes. This is not the case for the Ge/Si nanostructures subjected to thermal treatment. Here, improved structure quality together with high levels of uniformity of the size and shape is observed.