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Harder, Ross

Publications and source records attributed to Harder, Ross.

At least 73 records · Page 4

Utilizing broadband X-rays in a Bragg coherent X-ray diffraction imaging experiment

A method is presented to simplify Bragg coherent X-ray diffraction imaging studies of complex heterogeneous crystalline materials with a two-stage screening/imaging process that utilizes polychromatic and monochromatic coherent X-rays and is compatible with in situ sample environments. Coherent white-beam diffraction is used to identify an individual crystal particle or grain that displays desired properties within a larger population. A three-dimensional reciprocal-space map suitable for diffraction imaging is then measured for the Bragg peak of interest using a monochromatic beam energy scan that requires no sample motion, thus simplifying in situ chamber design. This approach was demonstrated with Au nanoparticles and will enable, for example, individual grains in a polycrystalline material of specific orientation to be selected, then imaged in three dimensions while under load.

36 MATERIALS SCIENCE↗

Novel silica stabilization method for the analysis of fine nanocrystals using coherent X-ray diffraction imaging

High-energy X-ray Bragg coherent diffraction imaging (BCDI) is a well established synchrotron-based technique used to quantitatively reconstruct the three-dimensional morphology and strain distribution in nanocrystals. The BCDI technique has become a powerful analytical tool for quantitative investigations of nanocrystals, nanotubes, nanorods and more recently biological systems. BCDI has however typically failed for fine nanocrystals in sub-100?nm size regimes ? a size routinely achievable by chemical synthesis ? despite the spatial resolution of the BCDI technique being 20?30?nm. The limitations of this technique arise from the movement of nanocrystals under illumination by the highly coherent beam, which prevents full diffraction data sets from being acquired. A solution is provided here to overcome this problem and extend the size limit of the BCDI technique, through the design of a novel stabilization method by embedding the fine nanocrystals into a silica matrix. Chemically synthesized FePt nanocrystals of maximum dimension 20?nm and AuPd nanocrystals in the size range 60?65?nm were investigated with BCDI measurement at beamline 34-ID-C of the APS, Argonne National Laboratory. Novel experimental methodologies to elucidate the presence of strain in fine nanocrystals are a necessary pre-requisite in order to better understand strain profiles in engineered nanocrystals for novel device development.

36 MATERIALS SCIENCE↗

Materials science in the time domain using Bragg coherent diffraction imaging

Materials are generally classified by a phase diagram which displays their properties as a function of external state variables, typically temperature and pressure. A new dimension that is relatively unexplored is time: a rich variety of new materials can become accessible in the transient period following laser excitation from the ground state. The timescale of nanoseconds to femtoseconds, is ripe for investigation using x-ray free-electron laser (XFEL) methods. There is no shortage of materials suitable for time-resolved materials-science exploration. Oxides alone represent most of the minerals making up the Earth's crust, catalysts, ferroelectrics, corrosion products and electronically ordered materials such as superconductors, to name a few. Some of the elements have metastable phase diagrams with predicted new phases. There are some examples known already: an oxide 'hidden phase' living only nanoseconds and an electronically ordered excited phase of fullerene C 60 , lasting only femtoseconds. In a completely general way, optically excited states of materials can be probed with Bragg coherent diffraction imaging, both below the damage threshold and in the destructive regime. Lastly, prospective methods for carrying out such XFEL experiments are discussed.

36 MATERIALS SCIENCE↗

Hard X-ray polarizer to enable simultaneous three-dimensional nanoscale imaging of magnetic structure and lattice strain

Recent progress in the development of dichroic Bragg coherent diffractive imaging, a new technique for simultaneous three-dimensional imaging of strain and magnetization at the nanoscale, is reported. This progress includes the installation of a diamond X-ray phase retarder at beamline 34-ID-C of the Advanced Photon Source. Here, the performance of the phase retarder for tuning X-ray polarization is demonstrated with temperature-dependent X-ray magnetic circular dichroism measurements on a gadolinium foil in transmission and on a Gd 5 Si 2 Ge 2 crystal in diffraction geometry with a partially coherent, focused X-ray beam. Feasibility tests for dichroic Bragg coherent diffractive imaging are presented. These tests include (1) using conventional Bragg coherent diffractive imaging to determine whether the phase retarder introduces aberrations using a nonmagnetic gold nanocrystal as a control sample, and (2) collecting coherent diffraction patterns of a magnetic Gd 5 Si 2 Ge 2 nanocrystal with left- and right-circularly polarized X-rays. Future applications of dichroic Bragg coherent diffractive imaging for the correlation of strain and lattice defects with magnetic ordering and inhomogeneities are considered.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Deformation Twinning of a Silver Nanocrystal under High Pressure

Within a high-pressure environment, crystal deformation is controlled by complex processes such as dislocation motion, twinning, and phase transitions, which change materials' microscopic morphology and alter their properties. Understanding a crystal's response to external stress provides a unique opportunity for rational tailoring of its functionalities. It is very challenging to track the strain evolution and physical deformation from a single nanoscale crystal under high-pressure stress. Here, we report an in situ three-dimensional mapping of morphology and strain evolutions in a single-crystal silver nanocube within a high-pressure environment using the Bragg Coherent Diffractive Imaging (CDI) method. We observed a continuous lattice distortion, followed by a deformation twining process at a constant pressure. The ability to visualize stress-introduced deformation of nanocrystals with high spatial resolution and prominent strain sensitivity provides an important route for interpreting and engineering novel properties of nanomaterials.

coherent diffractive imaging↗

Achieving Hard X-ray Nanofocusing Using a Wedged Multilayer Laue Lens

Here, we report on the fabrication and the characterization of a wedged multilayer Laue lens for x-ray nanofocusing. The lens was fabricated using a sputtering deposition technique, in which a specially designed mask was employed to introduce a thickness gradient in the lateral direction of the multilayer. X-ray characterization shows an efficiency of 27% and a focus size of 26 nm at 14.6 keV, in a good agreement with theoretical calculations. Our results indicate that the desired wedging is achieved in the fabricated structure. Furthermore, we anticipate that continuous development on wedged MLLs will advance x-ray nanofocusing optics to new frontiers and enrich capabilities and opportunities for hard X-ray microscopy.

42 ENGINEERING↗

Ptychographic x-ray imaging of surfaces on crystal truncation rod

Ptychography is a high-resolution imaging technique, which does not require lenses for image magnification and which provides phase contrast with high sensitivity. Here, we propose to use x-ray ptychography for the imaging of surface structure in crystalline samples. We show that ptychography can be used to image atomic step structures using coherent diffraction patterns recorded along the crystal truncation rod of a crystal surface. In a proof-of-concept experiment on a Pt (111) sample, we present ptychographic reconstructions showing features consistent with surface steps. Due to the penetration power of x-rays, this method could find interesting applications for the study of surface structures under buried interfaces or in harsh environments.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

In situ strain evolution during a disconnection event in a battery nanoparticle

Lithium ion batteries are the dominant form of energy storage in mobile devices, increasingly employed in transportation, and likely candidates for renewable energy storage and integration into the electrical grid. To fulfil their powerful potential, electrodes with increased capacity, faster charge rates, and longer cycle life must be developed. Understanding the mechanics and chemistry of individual nanoparticles under in situ conditions is a crucial step to improving performance and mitigating damage. Here we reveal three-dimensional strain evolution within a single nanoparticle of a promising high voltage cathode material, LiNi 0.5 Mn 1.5 O 4, under in situ conditions. The particle becomes disconnected during the second charging cycle. This is attributed to the formation of a cathode electrolyte interphase layer with slow ionic conduction. The three-dimensional strain pattern within the particle is independent of cell voltage after disconnection, indicating that the particle is unable to redistribute lithium within its volume or to its neighbours. Understanding the disconnection process at the single particle level and the equilibrium or non-equilibrium state of nanoparticles is essential to improving performance of current and future electrochemical energy storage system

Ulvestad, Andrew↗

Coherent X-ray diffraction imaging and characterization of strain in silicon-on-insulator nanostructures

Coherent X-ray diffraction imaging (CDI) has emerged in the last decade as a promising high resolution lens-less imaging approach for the characterization of various samples. It has made significant technical progress through developments in source, algorithm and imaging methodologies thus enabling important scientific breakthroughs in a broad range of disciplines. In this report, we will introduce the principles of forward scattering CDI and Bragg geometry CDI (BCDI), with an emphasis on the latter. BCDI exploits the ultra-high sensitivity of the diffraction pattern to the distortions of crystalline lattice. Its ability of imaging strain on the nanometer scale in three dimensions is highly novel. We will present the latest progress on the application of BCDI in investigating the strain relaxation behavior in nanoscale patterned strained silicon-on-insulator (sSOI) materials, aiming to understand and engineer strain for the design and implementation of new generation semiconductor devices.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Continuous scanning mode for ptychography

We outline how ptychographic imaging can be performed without the need for discrete scan positions. Through an idealized experiment, we demonstrate how a discrete-position scan regime can be replaced with a continuously scanned one with suitable modification of the reconstruction scheme based on coherent modes. The impact of this is that acquisition times can be reduced, significantly aiding ptychographic imaging with x rays, electrons, or visible light.

Clark, Jesse N.↗

Brownian motion studies of viscoelastic colloidal gels by rotational single particle tracking

Colloidal gels have unique properties due to a complex microstructure which forms into an extended network. Although the bulk properties of colloidal gels have been studied, there has been difficulty correlating those properties with individual colloidal dynamics on the microscale due to the very high viscosity and elasticity of the material. We utilize rotational X-ray tracking (RXT) to investigate the rotational motion of component crystalline colloidal particles in a colloidal gel of alumina and decanoic acid. Our investigation has determined that the high elasticity of the bulk is echoed by a high elasticity experienced by individual colloidal particles themselves but also finds an unexpected high degree of rotational diffusion, indicating a large degree of freedom in the rotational motion of individual colloids even within a tightly bound system.

36 MATERIALS SCIENCE↗