Single Alloy Nanoparticle X-Ray Imaging during a Catalytic Reaction

The imaging of active nanoparticles represents a milestone in decoding heterogeneous catalysts dynamics. We report the facet resolved, surface strain state of a single PtRh alloy nanoparticle on SrTiO3 determined by coherent x-ray diffraction imaging under catalytic reaction conditions. Density functional theory calculations allow us to correlate the facet surface strain state to its reaction environment dependent chemical composition. We find that the initially Pt terminated nanoparticle surface gets Rh enriched under CO oxidation reaction conditions. The local composition is facet orientation dependent and the Rh enrichment is non-reversible under subsequent CO reduction. Tracking facet resolved strain and composition under operando conditions is crucial for a rational design of more efficient heterogeneous catalysts with tailored activity, selectivity and lifetime.Comment: 15 pages, 4 figures, 32 reference

Time-Resolved in Situ Visualization of the Structural Response of Zeolites During Catalysis

Zeolites are three-dimensional aluminosilicates having unique properties from the size and connectivity of their sub-nanometer pores, the Si/Al ratio of the anionic framework, and the charge-balancing cations. The inhomogeneous distribution of the cations affects their catalytic performances because it influences the intra-crystalline diffusion rates of the reactants and products. However, the structural deformation regarding inhomogeneous active regions during the catalysis is not yet observed by conventional analytical tools. Here we employ in situ X-ray free electron laser-based time-resolved coherent X-ray diffraction imaging to investigate the internal deformations originating from the inhomogeneous Cu ion distributions in Cu-exchanged ZSM-5 zeolite crystals during the deoxygenation of nitrogen oxides with propene. We show that the interactions between the reactants and the active sites lead to an unusual strain distribution, confirmed by density functional theory simulations. These observations provide insights into the role of structural inhomogeneity in zeolites during catalysis and will assist the future design of zeolites for their applications

PyNX : high-performance computing toolkit for coherent X-ray imaging based on operators

International audienceThe open-source PyNX toolkit has been extended to provide tools for coherent X-ray imaging data analysis and simulation. All calculations can be executed on graphical processing units (GPUs) to achieve high-performance computing speeds. The toolkit can be used for coherent diffraction imaging (CDI), ptychography and wavefront propagation, in the far- or near-field regime. Moreover, all imaging operations (propagation, projections, algorithm cycles…) can be implemented in Python as simple mathematical operators, an approach which can be used to easily combine basic algorithms in a tailored chain. Calculations can also be distributed to multiple GPUs, e.g. for large ptychography data sets. Command-line scripts are available for on-line CDI and ptychography analysis, either from raw beamline data sets or using the coherent X-ray imaging data format

Surface and Interfacial Morphology of Bulk Heterojunction Layers in Organic Solar Cells with Solvent Additive

We study the surface and interfacial morphology of a bulk heterojunction (BHJ) layer with the solvent additive effect by using the X-ray reflectivity and the grazing incidence X-ray scattering techniques. The BHJ layer consists of poly(4,8-bis[(2-ethylhexyl)oxy]benzo[1,2-b:4,5-b???]dithiophene-2,6-diyl-alt-3-fluoro-2-[(2-ethylhexyl)carbonyl] thieno[3,4-b]thiophene-4,6-diyl) (PTB7) and [6,6]-phenyl C71-butyric acid methyl ester (PC71BM) deposited on a poly(3,4-ethylenedioxythiophene): poly(styrene sulfonate) (PEDOT:PSS) coated Si substrate. An interfacial layer with a low electron density is observed between the BHJ and PEDOT:PSS layers, which becomes less distinct when the additive 1,8-diiodooctane (DIO) is added to the film processing solvent. This result indicates that DIO causes PC71BM to become more uniformly distributed throughout the entire BHJ layer. The surface roughness of the BHJ significantly decreases with increasing addition of DIO. The understanding of the surface and interfacial morphology gives an important clue to improving the structures and efficiency

Precise wavefront characterization of X-ray optical elements using a laboratory source

Improvements in x-ray optics critically depend on the measurement of their optical performance. The knowledge of wavefront aberrations, for example, can be used to improve the fabrication of optical elements or to design phase correctors to compensate for these errors. At present, the characterization of such optics is made using intense x-ray sources, such as synchrotrons. However, the limited access to these facilities can substantially slow down the development process. Improvements in the brightness of lab-based x-ray micro-sources in combination with the development of new metrology methods, particularly ptychographic x-ray speckle tracking, enable characterization of x-ray optics in the lab with a precision and sensitivity not possible before. Here, we present a laboratory setup that utilizes a commercially available x-ray source and can be used to characterize different types of x-ray optics. The setup is used in our laboratory on a routine basis to characterize multilayer Laue lenses of high numerical aperture and other optical elements. This typically includes measurements of the wavefront distortions, optimum operating photon energy, and focal length of the lens. To check the sensitivity and accuracy of this laboratory setup, we compared the results to those obtained at the synchrotron and saw no significant difference. To illustrate the feedback of measurements on performance, we demonstrated the correction of the phase errors of a particular multilayer Laue lens using a 3D printed compound refractive phase plate

Cylindrical Reflex Triode Warm X-Ray Source

Cylindrical reflex triodes (CRTs) driven by a pulsed power generator can produce relatively low-endpoint X-ray spectra (~250 keV) that can be suitable for certain radiation-matter interaction studies. CRTs have several advantages over other reflex triode configurations, the most significant being the ability to operate multiple concentric CRTs, connected either in parallel or in series. Such configurations can result in increased X-ray output without increasing the endpoint or changing the pulsed-power generator. This article describes results from, and modeling of, experiments employing a single CRT and two CRTs in a series configuration. The modeling includes an analytic, physics-based model of CRT electrical operation; measured and calculated radiation distributions and spectra; and predicted effects of several configuration variations

Raw data repository for manuscript "Single Alloy Nanoparticle X-Ray Imaging during a Catalytic Reaction"

Raw data depository for https://arxiv.org/abs/2103.01573. Details with file information are given in the file description-of-datasets.pd

Robust Ptychographic X-ray Speckle Tracking with Multilayer Laue lenses

In recent years, X-ray speckle tracking techniques have emerged as viable tools for wavefront metrology and sample imaging applications, and have been actively developed for use at synchrotron light sources. Speckle techniques can recover an image free of aberrations and can be used to measure wavefronts with a high angular sensitivity. Since they are compatible with low-coherence sources they can be also used with laboratory X-ray sources. A new implementation of the ptychographic X-ray speckle tracking method, suitable for the metrology of highly divergent wavefields, such as those created by multilayer Laue lenses, is presented here. This new program incorporates machine learning techniques such as Huber and non-parametric regression and enables robust and quick wavefield measurements and data evaluation even for low brilliance X-ray beams, and the imaging of low-contrast samples. To realize this, a software suite was written in Python 3, with a C back-end capable of concurrent calculations for high performance. It is accessible as a Python module and is available as source code under Version 3 or later of the GNU General Public License