Characterization of Materials through High Resolution Coherent Imaging: High Resolution Characterization of Materials with Coherent Diffraction Imaging
Sponsored by: TMS Extraction and Processing Division, TMS Structural Materials Division, TMS: Advanced Characterization, Testing, and Simulation Committee, TMS: Materials Characterization Committee
Program Organizers: Richard Sandberg, Brigham Young University; Ross Harder, Argonne National Laboratory; Xianghui Xiao, Brookhaven National Laboratory; Brian Abbey, La Trobe University; Saryu Fensin, Los Alamos National Laboratory; Ana Diaz, Paul Scherrer Institute; Mathew Cherukara, Argonne National Laboratory
Monday 8:30 AM
March 20, 2023
Room: Aqua 310A
Location: Hilton
Session Chair: Ana Diaz, Swiss Light Source, Paul Scherrer Institute
8:30 AM Invited
Structural Evolution of Nanoparticles Under Realistic Conditions Observed with Bragg Coherent X-ray Imaging: Marie-Ingrid Richard1; Maxime Dupraz1; Corentin Chatelier1; Clément Atlan1; Sarah Yehya2; David Simonne2; Stéphane Labat3; Steven Leake4; Ewen Bellec4; Tobias Schulli4; Olivier Thomas3; Joel Eymery1; Eugen Rabkin5; 1CEA Grenoble; 2Synchrotron SOLEIL; 3IM2NP-CNRS; 4ESRF; 5Technion
The advent of the new 4th generation x-ray light sources represents an unprecedented opportunity to conduct in situ studies on the structure of nanoparticles during their operation. Here, we will illustrate how Bragg coherent x-ray imaging allows to image in three dimensions and at the nanoscale the strain and defect dynamics inside nanoparticles during heat treatment and catalytic reactions. This imaging technique can be coupled with molecular statics simulations to investigate the 3D strain and stress fields in nanoparticles. We will also discuss the possibility to enable extremely high-resolution and high-energy imaging with Bragg coherent x-ray diffraction at 4th generation x-ray light sources. Finally, we will highlight the potential of machine learning to predict characteristic structural features in nanocrystals just from their 3D Bragg coherent diffraction patterns.
9:00 AM
Nanoscale Imaging of Electrochemically-induced Strain Dynamics in a Locally Polarized Pt Grain: Dina Sheyfer1; Ruperto Mariano2; Tomoya Kawaguchi3; Wonsuk Cha1; Ross Harder1; Mathew Kanan4; Stephan Hruszkewycz1; Hoydoo You1; Matthew Highland1; 1Argonne National Laboratory; 2Massachusetts Institute of Technology; 3Tohoku University; 4Stanford University
Probing structural rearrangements in catalytic materials during electrocatalysis is challenging experimentally and further complicated by structural heterogeneities including crystalline defects, strain inhomogeneities, and variations in chemical composition. Nonetheless, in operando measurements are often the most direct ways to improve our understanding of catalytic reactions. To address this challenge, we demonstrate a new approach that combines a nanopipette electrochemical cell (NEC) with three-dimensional X-ray Bragg Coherent Diffractive Imaging (BCDI) to study how strain in a single Pt grain evolves in response to applied potential. During electrochemical polarization, in-situ BCDI measurements have revealed marked changes in surface strain arising from the Coulombic attraction between the electrode surface and the electrolyte ions in electrochemical double layers, while the strain in the bulk of the crystal remained unchanged. The concurrent surface redox reactions have a strong influence on the magnitude and nature of the strain dynamics under polarization.
9:20 AM
In Situ and Operando 3D Imaging of Pt and Pd Electrocatalytic Nanocrystals: Clement Atlan1; Corentin Chatelier1; Arnaud Viola2; Maxime Dupraz3; Isaac Martens4; Joël Eymery1; Frédéric Maillard2; Marie-Ingrid Richard1; 1French Alternative Energies and Atomic Energy Commission; 2Laboratory of Electrochemistry and Physical-Chemistry of Materials and Interfaces; 3French National Centre for Scientific Research; 4European Synchrotron Radiation Facility
Structural properties of transition metal are critical to understand the catalytic behavior of electrochemical processes. Here we show that Pt and Pd nanocrystals can be probed in situ and operando at the fourth generation Extremely Brilliant Source of ESRF by Bragg Coherent X-ray Diffraction Imaging. This lens-less technique enables determining the morphology as well as mapping the strain and displacement fields of such nanoparticles. By measuring the Pt 002 reflection we show evidence of heterogeneous and potential-dependent strain distribution between highly-coordinated ({100} and {111} facets) and under-coordinated atoms (edges and corners) as well as evidence of strain propagation from the surface to the bulk of the nanoparticle. This allows to unveil adsorption sites. We also demonstrate that the formation of highly strained palladium hydride nanocrystals can be tracked under potential control. Even though the beta phase comes and vanishes at relevant potentials, the nanocrystal does not recover its pristine morphology.
9:40 AM
Exploring the Formation of Superlattice in Metal Nanocrystals using Bragg Coherent X-ray Diffraction Imaging: Ericmoore Jossou1; Ana Suzana1; Longlong Wu1; Jiecheng Diao2; Tadesse Assefa3; Steven Leake4; Adam Gabriel5; Anton Schneider6; Kim Kisslinger1; Lin Shao5; Yongfeng Zhang6; Lynne Ecker1; Jian Gan7; Ian Robinson1; Simerjeet Gill1; 1Brookhaven National Laboratory; 2University College London; 3SLAC National Accelerator Laboratory; 4The European Synchrotron Facility; 5Texas A&M University; 6University of Wisconsin; 7Idaho National Laboratory
Self-organization of defects in materials can create novel physical properties with potential applications in electronics and nuclear energy systems. In our work, we studied the physical mechanism of self-organization of krypton gas bubbles in nanocrystalline palladium under ion implantation. The formation of superlattices is affected by surface defects sinks which are predominant in nanocrystals compared to bulk metals. Using Bragg coherent X-ray diffraction imaging and transmission electron microscope, we determined the structure of the nanocrystal with the resolution sufficient to resolve each palladium nanoparticle. The reconstructed electron density of the nanocrystal reveals its intrinsic structural heterogeneity, including local deviations of lattice parameters, and the presence of internal defects. Variation in strain and lattice parameters and distribution of defects as a function of implantation conditions and fundamental mechanisms of noble gas ordering in nanocrystals compared to the bulk counterpart will be discussed.
10:00 AM Break
10:20 AM Invited
Searching for Crystals, Twins, Peaks and Dislocations with BCDI: Anthony Rollett1; Yueheng Zhang1; Matthew Wilkin1; Robert Suter1; Nicholas Porter2; Richard Sandberg2; Wonsuk Cha3; Ross Harder3; Siddharth Maddali3; Stephan Hruszkewycz3; 1Carnegie Mellon University; 2Brigham Young University; 3Argonne National Lab
Bragg Coherent Diffraction Imaging (BCDI) has been available for several years and there is clear potential for investigating mesoscale phenomena in materials science. The current coherence lengths of roughly 1 micron has motivated samples as varied as de-wetted films, deposits in vias and liftouts from bulk polycrystalline materials. Studying dislocation-boundary interactions has motivated multi-peak and more recently multi-grain reconstructions. It has also prompted development of polycrystal mapping, whether it be HEDM at high energies or Laue diffraction at medium energies. Recent results suggest that a multi-grain reconstruction of a matrix-twin-matrix 3-grain oligocrystal of gold on strontium titanate yields reasonable results that moreover suggest the presence of a dislocation in one of the grains.
10:50 AM Invited
High-speed Free-run Ptychography at the Australian Synchrotron: Cameron Kewish1; 1Australian Nuclear Science and Technology Organization
The X-ray fluorescence microscopy (XFM) beamline at the Australian Synchrotron has recently implemented ptychography as a user experiment [1]. The fast-scanning coherent X-ray diffraction microscopy method benefits from the optimized high-speed “megapixels per hour” scanning architecture developed for XFM, and the dead-time free noiseless photon-counting operation of a hybrid pixel detector. Free-run data collection is demonstrated to improve the quality and reliability of ptychography image reconstruction. This makes ptychography compatible as a simultaneous experiment to XFM mapping. Extremely high scan area coverage up to 140 µm2 s-1 has been achieved at up to 250 µm s-1 scan velocity, over regions up to 352 000 mm2, with a reconstructed image resolution gain of 13× compared to the beam size. The combination of these methods provides unique morphological context for elemental and chemical information, enabling novel scientific outcomes. [1] M. W. M. Jones, et al. J. Synchrotron Rad. 29, 480-487 (2022).
11:20 AM
Catalytic Properties at the Nanoscale Probed by Coherent Diffraction Imaging: David Simonne1; Andrea Resta1; Alessandro Coati; Alina Vlad1; Benjamin Voisin1; Yves Garreau1; Corentin Chatelier2; Maxime Dupraz3; Marie-Ingrid Richard2; 1Synchrotron SOLEIL; 2CEA Grenoble; 3ESRF
The multi-environment diffractometer at SixS (Synchrotron SOLEIL) has recently been updated for coherent diffraction imaging via a new set of coherence optics. The XCAT gas flow reactor allows us to perform near ambient pressure measurements under variant gas flows, pressure, and temperature, followed by mass spectroscopy. A new data analysis workflow favouring reproducibility and compatible with computing clusters allows us to perform real time data analysis. We perform Bragg coherent diffraction imaging measurements of isolated Pt nanoparticles that act as model catalysts during the oxidation of ammonia for specific gas and temperature conditions linked to product selectivity.By following the evolution of multiple parameters in 3D (size, strain, shape, re-faceting) of the reconstructed nanoparticle, we gain important insight into the structure dependence of the catalytic properties of the nanoparticle; this, in return, provides information on the catalytically active facets and on the deactivation process of the particles.
11:40 AM
In Situ Bragg Coherent X-ray Diffraction Imaging Studies: David Yang1; Nicholas Phillips2; Kay Song1; Guanze He1; Clara Barker1; Wonsuk Cha3; Ross Harder3; Wenjun Liu3; Dina Sheyfer3; Felix Hofmann1; 1University of Oxford; 2Paul Scherrer Institute; 3Argonne National Laboratory
Lattice defects control the properties of crystalline materials and can be engineered to induce specific material properties. Understanding how defects evolve in response to an external environment is paramount for selecting and designing materials. Here I will discuss three in situ BCDI experiments: annealing of focused ion beam damaged gold microcrystals, corrosion of a Co-Fe microcrystal alloy in hydrochloric acid, and electrochemical Hydrogen charging in a stainless-steel grain. For annealing, we note the evolution in strain and crystal morphology driven by gold atom migration and observe how defects are removed from the crystal. For corrosion, we determine that the more strained surface layers are corroded first, and note a facet-dependent corrosion rate based on exposure to the flowing acid. Finally, I will discuss nanoscale strain evolution as a result of Hydrogen charging and its implications on the properties of stainless-steel.
12:00 PM
Internal Strain Changes of Pt Nanoparticles in Response to the High Pressure in Diamond-anvil Cell: Stephane Labat1; Sarah Yehya1; Marie-Ingrid Richard2; Felisa Berenguer3; Pierre Fertey3; Steven Leake4; Bjorn Wehinger4; Mor Levi5; Eugen Rabkin5; Mohamed Mezouar4; 1AMU-CNRS; 2CEA; 3SOLEIL; 4ESRF; 5TECHNION
Tremendous novel properties and new forms of materials have been revealed exclusively under high-pressure. Measuring and understanding the internal strain changes in response to the external pressure produces critical information to unveil the origin of unconventional behavior of crystalline materials in high-pressure environments. We have performed in-situ experiments in diamond-anvil cells (DACs) combining high-pressure and Bragg Coherent Diffraction Imaging. The 33.169 keV incident X-ray beam has been focused to a size of 1 x 1 µm² using a KB mirror and the diffracted X-rays have been recorded by an Eiger9M detector installed at 2 m from the sample. The strain evolution and physical deformation from a single nanoscale crystal of Platinum have been tracked for 5 different levels of pressure, ranging between 0.6 and 7 GPa. It evidences the ability to visualize large inhomogeneity with high spatial resolution (15 nm) and prominent strain sensitivity (0.02 %).
12:20 PM
Rationalization of CO2 Adsorption on Ni nanocrystals using Bragg Coherent X-ray Imaging: Corentin Chatelier1; Clément Atlan1; David Simonne2; Joël Eymery1; Marie-Ingrid Richard1; 1CEA Grenoble; 2Synchrotron SOLEIL
Every year, human activities release billions of CO2 into the atmosphere, causing global climate change due its greenhouse effect. An approach to prevent this issue is the chemical recycling of CO2 through its hydrogenation into value-added products. Ni-based catalysts are the most widely used due to their low-cost and high selectivity. As the thermodynamic feasibility of the conversion of CO2 to methane and methanol is highly depending on the partial pressure of the reactants, it is of interest to evaluate the effect of the reaction conditions on the strain evolution. In this regard, the surface strain of a single 300 nm Ni nanocrystal is probed using in situ Bragg Coherent X-ray Imaging under different partial pressures of CO2 (50 to 250 mbar) at the fourth generation Extremely Brilliant Source of ESRF. This reveals important and reversible strain signatures. This allows to gather new insights into possible adsorption and reaction mechanisms.