S. O. Hruszkewycz

Quantitative nanoscale imaging of lattice distortions in epitaxial semiconductor heterostructures using nanofocused X-ray Bragg projection ptychography.

We imaged nanoscale lattice strain in a multilayer semiconductor device prototype with a new X-ray technique, nanofocused Bragg projection ptychography. Applying this technique to the epitaxial stressor layer of a SiGe-on-SOI structure, we measured the internal lattice behavior in a targeted region of a single device and demonstrated that its internal strain profile consisted of two competing lattice distortions. These results provide the strongest nondestructive test to date of continuum modeling predictions of nanoscale strain distributions.

High contrast x-ray speckle from atomic-scale order in liquids and glasses

The availability of ultrafast pulses of coherent hard x rays from the Linac Coherent Light Source opens new opportunities for studies of atomic-scale dynamics in amorphous materials. Here, we show that single ultrafast coherent x-ray pulses can be used to observe the speckle contrast in the high-angle diffraction from liquid Ga and glassy Ni(2)Pd(2)P and B(2)O(3). We determine the thresholds above which the x-ray pulses disturb the atomic arrangements. Furthermore, high contrast speckle is observed in scattering patterns from the glasses integrated over many pulses, demonstrating that the source and optics are sufficiently stable for x-ray photon correlation spectroscopy studies of dynamics over a wide range of time scales.

Octahedral rotations in strained LaAlO3/SrTiO3 (001) heterostructures

Many complex oxides display an array of structural instabilities often tied to altered electronic behavior. For oxide heterostructures, several different interfacial effects can dramatically change the nature of these instabilities. Here, we investigate LaAlO3/SrTiO3 (001) heterostructures using synchrotron x-ray scattering. We find that when cooling from high temperature, LaAlO3 transforms from the Pm3¯m to the Imma phase due to strain. Furthermore, the first 4 unit cells of the film adjacent to the substrate exhibit a gradient in rotation angle that can couple with polar displacements in films thinner than that necessary for 2D electron gas formation.

Single shot speckle and coherence analysis of the hard X-ray free electron laser LCLS

The single shot based coherence properties of hard x-ray pulses from the Linac Coherent Light Source (LCLS) were measured by analyzing coherent diffraction patterns from nano-particles and gold nanopowder. The intensity histogram of the small angle x-ray scattering ring from nano-particles reveals the fully transversely coherent nature of the LCLS beam with a number of transverse mode 〈Ms〉 = 1.1. On the other hand, the speckle contrasts measured at a large wavevector yields information about the longitudinal coherence of the LCLS radiation after a silicon (111) monochromator. The quantitative agreement between our data and the simulation confirms a mean coherence time of 2.2 fs and a x-ray pulse duration of 29 fs. Finally the observed reduction of the speckle contrast generated by x-rays with pulse duration longer than 30 fs indicates ultrafast dynamics taking place at an atomic length scale prior to the permanent sample damage.

X-ray nanodiffraction of tilted domains in a poled epitaxial BiFeO3 thin film

We present measurements of crystallographic domain tilts in a (001) BiFeO3 thin film using focused beam x-ray nanodiffraction. Films were ferroelectrically pre-poled with an electric field orthogonal and parallel to as-grown tilt domain stripes. The tilt domains, associated with higher energy (010) vertical twin walls, displayed different nanostructural responses based on the poling orientation. Specifically, an electric field applied perpendicular to the as-grown domain stripe allowed the domain tilts and associated vertical twin walls to persist. The result demonstrates that thin film ferroelectric devices can be designed to maintain unexpected domain morphologies in working poled environments.

Phase stabilization of δ-Bi2O3 nanostructures by epitaxial growth onto single crystal SrTiO3 or DyScO3 substrates

We observe that the high-temperature δ-phase of Bi2O3 is stabilized to room temperature by the epitaxial growth of nanostructures onto either (001)-oriented SrTiO3 or (001)p-oriented DyScO3 single crystal substrates. In addition, the morphology can be controlled by the miscut of the substrate. Synchrotron x-ray scattering observations at controlled temperatures and oxygen partial pressures reveal that the δ-Bi2O3 nanostructures are coherently strained to the substrates at room temperature. Annealing the nanostructures at 600 °C causes gradual conversion of the (001)-oriented δ-phase to an unidentified strain-relaxed phase.

Framework for three-dimensional coherent diffraction imaging by focused beam x-ray Bragg ptychography

We present the framework for convergent beam Bragg ptychography, and, using simulations, we demonstrate that nanocrystals can be ptychographically reconstructed from highly convergent x-ray Bragg diffraction. The ptychographic iterative engine is extended to three dimensions and shown to successfully reconstruct a simulated nanocrystal using overlapping raster scans with a defocused curved beam, the diameter of which matches the crystal size. This object reconstruction strategy can serve as the basis for coherent diffraction imaging experiments at coherent scanning nanoprobe x-ray sources.

Measuring Three-Dimensional Strain and Structural Defects in a Single InGaAs Nanowire Using Coherent X-ray Multiangle Bragg Projection Ptychography

III-As nanowires are candidates for near-infrared light emitters and detectors that can be directly integrated onto silicon. However, nanoscale to microscale variations in structure, composition, and strain within a given nanowire, as well as variations between nanowires, pose challenges to correlating microstructure with device performance. In this work, we utilize coherent nanofocused X-rays to characterize stacking defects and strain in a single InGaAs nanowire supported on Si. By reconstructing diffraction patterns from the 21̅1̅0 Bragg peak, we show that the lattice orientation varies along the length of the wire, while the strain field along the cross-section is largely unaffected, leaving the band structure unperturbed. Diffraction patterns from the 011̅0 Bragg peak are reproducibly reconstructed to create three-dimensional images of stacking defects and associated lattice strains, revealing sharp planar boundaries between different crystal phases of wurtzite (WZ) structure that contribute to charge carrier scattering. Phase retrieval is made possible by developing multiangle Bragg projection ptychography (maBPP) to accommodate coherent nanodiffraction patterns measured at arbitrary overlapping positions at multiple angles about a Bragg peak, eliminating the need for scan registration at different angles. The penetrating nature of X-ray radiation, together with the relaxed constraints of maBPP, will enable the in operando imaging of nanowire devices.

The effect of exit beam phase aberrations on parallel beam coherent x-ray reconstructions.

Diffraction artifacts from imperfect x-ray windows near the sample are an important consideration in the design of coherent x-ray diffraction measurements. In this study, we used simulated and experimental diffraction patterns in two and three dimensions to explore the effect of phase imperfections in a beryllium window (such as a void or inclusion) on the convergence behavior of phasing algorithms and on the ultimate reconstruction. A predictive relationship between beam wavelength, sample size, and window position was derived to explain the dependence of reconstruction quality on beryllium defect size. Defects corresponding to this prediction cause the most damage to the sample exit wave and induce signature error oscillations during phasing that can be used as a fingerprint of experimental x-ray window artifacts. The relationship between x-ray window imperfection size and coherent x-ray diffractive imaging reconstruction quality explored in this work can play an important role in designing high-resolution in situ coherent imaging instrumentation and will help interpret the phasing behavior of coherent diffraction measured in these in situ environments.

Towards ultrafast dynamics with split-pulse X-ray photon correlation spectroscopy at free electron laser sources

One of the important challenges in condensed matter science is to understand ultrafast, atomic-scale fluctuations that dictate dynamic processes in equilibrium and non-equilibrium materials. Here, we report an important step towards reaching that goal by using a state-of-the-art perfect crystal based split-and-delay system, capable of splitting individual X-ray pulses and introducing femtosecond to nanosecond time delays. We show the results of an ultrafast hard X-ray photon correlation spectroscopy experiment at LCLS where split X-ray pulses were used to measure the dynamics of gold nanoparticles suspended in hexane. We show how reliable speckle contrast values can be extracted even from very low intensity free electron laser (FEL) speckle patterns by applying maximum likelihood fitting, thus demonstrating the potential of a split-and-delay approach for dynamics measurements at FEL sources. This will enable the characterization of equilibrium and, importantly also reversible non-equilibrium processes in atomically disordered materials.X-ray photon correlation spectroscopy has been mainly used to measure slow dynamics using synchrotron sources. Here the authors demonstrate the split-and- delay pulse set-up to study nanosecond dynamics of gold nanoparticles using XPCS with free electron laser pulses.