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Fuoss, P. H.

Publications and source records attributed to Fuoss, P. H..

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.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Island dynamics and anisotropy during vapor phase epitaxy of m-plane GaN

Using in situ grazing-incidence x-ray scattering, we have measured the diffuse scattering from islands that form during layer-by-layer growth of GaN by metal-organic vapor phase epitaxy on the (1010) m-plane surface. The diffuse scattering is extended in the (0001) in-plane direction in reciprocal space, indicating a strong anisotropy with islands elongated along [1210] and closely spaced along [0001]. This is confirmed by atomic force microscopy of a quenched sample. Islands were characterized as a function of growth rate F and temperature. The island spacing along [0001] observed during the growth of the first monolayer obeys a power-law dependence on growth rate F-n, with an exponent n = 0:25 + 0.02. The results are in agreement with recent kinetic Monte Carlo simulations, indicating that elongated islands result from the dominant anisotropy in step edge energy and not from surface diffusion anisotropy. The observed power-law exponent can be explained using a simple steady-state model, which gives n = 1/4.

36 MATERIALS SCIENCE↗

In-situ synchrotron x-ray studies of the microstructure and stability of In 2 O 3 epitaxial films

We report on the synthesis, stability, and local structure of In2O3 thin films grown via rf-magnetron sputtering and characterized by in-situ x-ray scattering and focused x-ray nanodiffraction. We find that In2O3 deposited onto (0 0 1)-oriented single crystal yttria-stabilized zirconia substrates adopts a Stranski-Krastanov growth mode at a temperature of 850 degrees C, resulting in epitaxial, truncated square pyramids with (1 1 1) side walls. We find that at this temperature, the pyramids evaporate unless they are stabilized by a low flux of In2O3 from the magnetron source. We also find that the internal lattice structure of one such pyramid is made up of differently strained volumes, revealing local structural heterogeneity that may impact the properties of In2O3 nanostructures and films.

36 MATERIALS SCIENCE↗

In situ study of annealing-induced strain relaxation in diamond nanoparticles using Bragg coherent diffraction imaging

Here, we observed changes in morphology and internal strain state of commercial diamond nanocrystals during high-temperature annealing. Three nanodiamonds were measured with Bragg coherent x-ray diffraction imaging, yielding three-dimensional strain-sensitive images as a function of time/temperature. Up to temperatures of 800 °C, crystals with Gaussian strain distributions with a full-width-at-half-maximum of less than 8 × 10 –4 were largely unchanged, and annealing-induced strain relaxation was observed in a nanodiamond with maximum lattice distortions above this threshold. X-ray measurements found changes in nanodiamond morphology at temperatures above 600 °C that are consistent with graphitization of the surface, a result verified with ensemble Raman measurements.

36 MATERIALS SCIENCE↗

Three Dimensional Variable-Wavelength X-Ray Bragg Coherent Diffraction Imaging

Here, we present and demonstrate a formalism by which three-dimensional (3D) Bragg x-ray coherent diffraction imaging (BCDI) can be implemented without moving the sample by scanning the energy of the incident x-ray beam. This capability is made possible by introducing a 3D Fourier transform that accounts for x-ray wavelength variability. We also demonstrate the approach by inverting coherent Bragg diffraction patterns from a gold nanocrystal measured with an x-ray energy scan. Furthermore, variable-wavelength BCDI will expand the breadth of feasible in situ 3D strain imaging experiments towards more diverse materials environments, especially where sample manipulation is difficult.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

High-resolution three-dimensional structural microscopy by single-angle Bragg ptychography

Coherent X-ray microscopy by phase retrieval of Bragg diffraction intensities enables lattice distortions within a crystal to be imaged at nanometre-scale spatial resolutions in three dimensions. While this capability can be used to resolve structure–property relationships at the nanoscale under working conditions, strict data measurement requirements can limit the application of current approaches. Here, in this work, we introduce an efficient method of imaging three-dimensional (3D) nanoscale lattice behaviour and strain fields in crystalline materials with a methodology that we call 3D Bragg projection ptychography (3DBPP). This method enables 3D image reconstruction of a crystal volume from a series of two-dimensional X-ray Bragg coherent intensity diffraction patterns measured at a single incident beam angle. Structural information about the sample is encoded along two reciprocal-space directions normal to the Bragg diffracted exit beam, and along the third dimension in real space by the scanning beam. Finally, we present our approach with an analytical derivation, a numerical demonstration, and an experimental reconstruction of lattice distortions in a component of a nanoelectronic prototype device.

36 MATERIALS SCIENCE↗

Structural sensitivity of x-ray Bragg projection ptychography to domain patterns in epitaxial thin films

Bragg projection ptychography (BPP) is a coherent diffraction imaging technique capable of mapping the spatial distribution of the Bragg structure factor in nanostructured thin films. Here, we show that, because these images are projections, the structural sensitivity of the resulting images depends on the film thickness and the aspect ratio and orientation of the features of interest and that image interpretation depends on these factors. Lastly, we model changes in contrast in the BPP reconstructions of simulated PbTiO 3 ferroelectric thin films with meandering 180° stripe domains as a function of film thickness, discuss their origin, and comment on the implication of these factors on the design of BPP experiments of general nanostructured films.

36 MATERIALS SCIENCE↗