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At least 775 records · Page 43
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Pair distribution function analysis of discrete nanomaterials in PDFgui

Pair distribution functions (PDFs) are a leading tool for atomic structure analysis of nanomaterials. However, the most widely used programs for refining atomic structure against PDF data are based on extended crystallographic models, which cannot be applied to discrete, whole nanoparticles. Furthermore, this work describes a straightforward approach to simulate and refine atomistic models of discrete clusters and nanoparticles employing widely used PDF modelling programs such as PDFgui that utilize extended crystallographic models. In this approach, the whole particle to be modelled is contained within an expanded, and otherwise empty, unit cell that is sufficiently large to avoid correlations between atoms in neighbouring unit cells over the r range analyzed. The PDF of the particle is simulated as a composite using two conventional `phases': one that calculates the atom–atom correlations and one that approximates the local number density. This approach is first validated for large nanoparticles that are well modelled by a conventional shape factor model, and then applied to simulate the PDF of discrete particles and low-dimensional materials (graphene and MXene) and to model the experimental PDF data for single-layer FeS nanosheets. A comparison of this approach with the DiffPy-CMI program, which calculates the PDF of discrete species, shows that the composite modelling approach is equally or more accurate. Example input files for implementing this approach within PDFgui and TOPAS, and recommendations for selecting model parameters for reliable application of this refinement strategy, are provided.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Pair distribution function analysis of nano-object assemblies

The atomic pair distribution function (aPDF) analysis technique, also known as the total scattering method, which considers both Bragg and diffuse scattering, has been used extensively to probe local atomic arrangements in crystalline and disordered materials. In contrast, there have been limited applications of the PDF in self-assembled nanomaterials, which represent a class of materials built from nanoscale objects, such as nano-colloids, micelles and proteins. As distinguished from atoms, nano-objects have polydispersity in size and shape, and such form-factor effects complicate the application of PDF analysis to nano-systems. Here, in this paper, the application of the PDF is extended to spherical nano-object assemblies and the formulae for the nano-PDF (nPDF) are derived, showing some differences from the aPDF. By numerical simulations, the properties of the nPDF (peak broadening and pattern profile) are studied systematically as a function of structural features, such as nano-object parameters (size and size polydispersity) and assembly structural features (size, shape, structure type and lattice disorder), and of data processing parameters ( q cut-off and `missing' data in ultra-small-angle regions). The nPDF analysis method is found to provide an effective route to revealing not only nanoscale but also mesoscale structural properties, for example the morphology of a nano-assembly.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2025

Solving disorder in (3D) real space: a comparative study of the three-dimensional difference pair distribution function and atomic resolution holography reconstructions

The quantitative analysis of local ordering principles in disordered crystalline systems has gained much attention over the past few years, as it is often considered crucial for optimizing material functionality. This development has been driven by significant advancements in computational and experimental methods, which have led to the establishment and widespread use of various analytical techniques. In this study, we perform model calculations to compare the effectiveness of atomic resolution holography and three-dimensional difference pair distribution function analysis (3D-ΔPDF). Using Cu 3 Au as a model system, we demonstrate an approach to derive local order parameters quantitatively and show that both techniques are well suited to quantifying chemical short-range order correlations and local bond-distance variations. By evaluating the strengths and limitations of both techniques, we advocate for their combined use to solve complex short-range order problems accurately.

3D-ΔPDF↗
DOE OSTI2022

Real-space texture and pole-figure analysis using the 3D pair distribution function on a platinum thin film

An approach is described for studying texture in nanostructured materials. The approach implements the real-space texture pair distribution function (PDF), txPDF, laid out by Gong & Billinge {(2018). arXiv:1805.10342 [cond-mat]}. It is demonstrated on a fiber-textured polycrystalline Pt thin film. The approach uses 3D PDF methods to reconstruct the orientation distribution function of the powder crystallites from a set of diffraction patterns, taken at different tilt angles of the substrate with respect to the incident beam, directly from the 3D PDF of the sample. A real-space equivalent of the reciprocal-space pole figure is defined in terms of interatomic vectors in the PDF and computed for various interatomic vectors in the Pt film. Furthermore, it is shown how a valid isotropic PDF may be obtained from a weighted average over the tilt series, including the measurement conditions for the best approximant to the isotropic PDF from a single exposure, which for the case of the fiber-textured film was in a nearly grazing incidence orientation of ∼10°. Finally, an open-source Python software package, FouriGUI , is described that may be used to help in studies of texture from 3D reciprocal-space data, and indeed for Fourier transforming and visualizing 3D PDF data in general.

3D pair distribution functions↗
DOE OSTI2022

Refining perovskite structures to pair distribution function data using collective Glazer modes as a basis

Structural modelling of octahedral tilts in perovskites is typically carried out using the symmetry constraints of the resulting space group. In most cases, this introduces more degrees of freedom than those strictly necessary to describe only the octahedral tilts. It can therefore be a challenge to disentangle the octahedral tilts from other structural distortions such as cation displacements and octahedral distortions. This paper reports the development of constraints for modelling pure octahedral tilts and implementation of the constraints in diffpy-CMI, a powerful package to analyse pair distribution function (PDF) data. The model in the program allows features in the PDF that come from rigid tilts to be separated from non-rigid relaxations, providing an intuitive picture of the tilting. The model has many fewer refinable variables than the unconstrained space group fits and provides robust and stable refinements of the tilt components. It further demonstrates the use of the model on the canonical tilted perovskite CaTiO 3 which has the known Glazer tilt system α + β – β – . The Glazer model fits comparably to the corresponding space-group model Pnma below r = 14 Å and becomes progressively worse than the space-group model at higher r due to non-rigid distortions in the real material.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Towards the extraction of the crystal cell parameters from pair distribution function profiles

The approach based on atomic pair distribution function (PDF) has revolutionized structural investigations by X-ray/electron diffraction of nano or quasi-amorphous materials, opening up the possibility of exploring short-range order. However, the ab initio crystal structural solution by the PDF is far from being achieved due to the difficulty in determining the crystallographic properties of the unit cell. A method for estimating the crystal cell parameters directly from a PDF profile is presented, which is composed of two steps: first, the type of crystal cell is inferred using machine-learning approaches applied to the PDF profile; second, the crystal cell parameters are extracted by means of multivariate analysis combined with vector superposition techniques. The procedure has been validated on a large number of PDF profiles calculated from known crystal structures and on a small number of measured PDF profiles. The lattice determination step has been benchmarked by a comprehensive exploration of different classifiers and different input data. The highest performance is obtained using the k -nearest neighbours classifier applied to whole PDF profiles. Descriptors calculated from the PDF profiles by recurrence quantitative analysis produce results that can be interpreted in terms of PDF properties, and the significance of each descriptor in determining the prediction is evaluated. The cell parameter extraction step depends on the cell metric rather than its type. Monometric, dimetric and trimetric cells have top-1 estimates that are correct 40, 20 and 5% of the time, respectively. Promising results were obtained when analysing real nanocrystals, where unit cells close to the true ones are found within the top-1 ranked solution in the case of monometric cells and within the top-6 ranked solutions in the case of dimetric cells, even in the presence of a crystalline impurity with a weight fraction up to 40%.

36 MATERIALS SCIENCE↗
DOE OSTI2021

A cloud platform for atomic pair distribution function analysis: PDFitc

A cloud web platform for analysis and interpretation of atomic pair distribution function (PDF) data ( PDFitc ) is described. The platform is able to host applications for PDF analysis to help researchers study the local and nanoscale structure of nanostructured materials. The applications are designed to be powerful and easy to use and can, and will, be extended over time through community adoption and development. The currently available PDF analysis applications, structureMining, spacegroupMining and similarityMapping , are described. In the first and second the user uploads a single PDF and the application returns a list of best-fit candidate structures, and the most likely space group of the underlying structure, respectively. In the third, the user can upload a set of measured or calculated PDFs and the application returns a matrix of Pearson correlations, allowing assessment of the similarity between different data sets. structureMining is presented here as an example to show the easy-to-use workflow on PDFitc . In the future, as well as using the PDFitc applications for data analysis, it is hoped that the community will contribute their own codes and software to the platform.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2023

Entangled Photon Pair Source Demonstrator Using the Quantum Instrumentation Control Kit System

Here, we report the first demonstration of using the Quantum Instrumentation and Control Kit (QICK) system on RFSoC-FPGA technology to drive the electro-optic intensity modulator that generate time-bin entangled photon pairs and to detect the photon signals. With the QICK system, we achieve high levels of performance metrics including coincidence-to-accidental ratio exceeding 150, and entanglement visibility exceeding 95%, consistent with performance metrics achieved using conventional waveform generators. We also demonstrate simultaneous detector readout using the digitization functional of QICK, achieving internal system synchronization time resolution of 3.2 ps. The work reported in this paper represents an explicit demonstration of the feasibility for replacing commercial waveform generators and time taggers with RFSoC-FPGA technology in the operation of a quantum network, representing a cost reduction of more than an order of magnitude.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2019

Total-scattering pair-distribution function analysis of zinc from high-energy synchrotron data

The crystal structure of zinc metal deviates from the ideal hexagonal close packing structure by a significantly increased axial ratio (c/a). The local atomic structure of zinc metal is investigated using the total scattering atomic pair distribution function (PDF) analysis based on X-ray powder diffraction data collected at ambient conditions. The X-ray total scattering PDF analysis confirms that the crystal structure of zinc can be described in terms of wurtzite structure, but with an anomalously atomic displacement parameters U 33 , indicating a significant displacement disorder along the c-axis. For the long r-range PDF refinements, the thermal motion of zinc shows a notable anisotropy as expressed by the ratio U 33 /U 11 of 2.5 at ambient conditions. This average distortion level along the c-axis, was not reflected locally for the features below 5.0 Å as it fits the high r region. Based on PDF refinements over different r-ranges, we measure an interesting increase of the U 33 value with decreasing the r-range of the refinement. Finally, this suggests that the local structure features in zinc metal differ from the average structure ones.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Functional Ion Pair Receptors Targeting Cesium, Lithium, Sulfate, and Uranyl (Final Technical Report)

The major goal of this project was the synthesis and study of receptors for key ions of interest to the DOE mission, namely cesium, lithium, sulfate, hydroxide, carbon dioxide/bicarbonate, and early actinides. The work, fundamental in nature, had as its objective achieving an increased understanding of how changes in receptor design could be used to optimize binding energies, ion specificity, complex structure, extraction efficiency, and substrate release. Within this broad paradigm, particular emphasis was placed on systems that could be used to sense the cesium cation in mixed aqueous media and act as extractants for the lithium cation and, separately, the carbon dioxide/bicarbonate and hydroxide anions in the form of ion pairs likely to be encountered under conditions of putative use in the field. The development of new nitrogen-rich ligands that act as receptors for early, high-valent actinide cations was also a major point of emphasis. The first in-plane actinide complexes were synthesized using a hexa-aza porphyrin analogue. The complexes exhibited an increase in the ligand–metal bonding covalency on passing from thorium(IV) to uranium(IV) to neptunium(IV) and illustrates how the use of appropriate porphyrinoid-like ligands could be used to modulate the covalency interactions between an f-element metal center and a ligand.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Metal-Organic Frameworks (MOFs) Containing Frustrated Lewis Pairs (FLP) for H 2 Storage at Ambient Temperature

This final technical report summarizes the key accomplishments of the HyMarc Seedling project to develop new materials based on metal-organic framework (MOF) incorporated with frustrated Lewis pairs (FLP) termed as FLP@MOF, as next-generation of hydrogen storage sorbent that can meet or exceed DOE’s 2025 performance target of hydrogen storage gravimetric density of 5.5 wt.% and volumetric density of 0.040 kg H 2 /L. The project was carried out by the PI Shengqian Ma at the University of North Texas (UNT) along with Argonne National Laboratory (ANL) to develop FLP@MOF systems that exhibit high hydrogen storage capacity at ambient temperature under pressure <100 bar, as well as to obtain improved fundamental understanding of hydrogen adsorption mechanism in FLP@MOF system.

08 HYDROGEN↗
DOE OSTI2021

Orbital Selectivity in Electron Correlations and Superconducting Pairing of Iron-Based Superconductors

Electron correlations play a central role in iron-based superconductors. In these systems, multiple Fe 3 d -orbitals are active in the low-energy physics, and they are not all degenerate. For these reasons, the role of orbital-selective correlations has been an active topic in the study of the iron-based systems. In this article, we survey the recent developments on the subject. For the normal state, we emphasize the orbital-selective Mott physics that has been extensively studied, especially in the iron chalcogenides, in the case of electron filling n ∼ 6 . In addition, the interplay between orbital selectivity and electronic nematicity is addressed. For the superconducting state, we summarize the initial ideas for orbital-selective pairing and discuss the recent explosive activities along this direction. We close with some perspectives on several emerging topics. These include the evolution of the orbital-selective correlations, magnetic and nematic orders, and superconductivity as the electron filling factor is reduced from 6 to 5, as well as the interplay between electron correlations and topological band structure in iron-based superconductors.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Using Complementary Methods of Synchrotron Radiation Powder Diffraction and Pair Distribution Function to Refine Crystal Structures with High Quality Parameters—A Review

Determination of the atomic-scale structures of certain fine-grained minerals using single-crystal X-ray diffraction (XRD) has been challenging because they commonly occur as submicron and nanocrystals in the geological environment. Synchrotron powder diffraction and scattering techniques are useful complementary methods for studying this type of minerals. In this review, we discussed three example studies investigated by combined methods of synchrotron radiation XRD and pair distribution function (PDF) techniques: (1) low-temperature cristobalite; (2) kaolinite; and (3) vernadite. Powder XRD is useful to determine the average structure including unit-cell parameters, fractional atomic coordinates, occupancies and isotropic atomic displacement parameters. X-ray/Neutron PDF methods are sensitive to study the local structure with anisotropic atomic displacement parameters (ADP). The results and case studies suggest that the crystal structure and high-quality ADP values can be obtained using the combined methods. The method can be useful to characterize crystals and minerals that are not suitable for single-crystal XRD.

58 GEOSCIENCES↗
DOE OSTI2021

Crystal Structure of Moganite and Its Anisotropic Atomic Displacement Parameters Determined by Synchrotron X-ray Diffraction and X-ray/Neutron Pair Distribution Function Analyses

The crystal structure of moganite from the Mogán formation on Gran Canaria has been re-investigated using high-resolution synchrotron X-ray diffraction (XRD) and X-ray/neutron pair distribution function (PDF) analyses. Our study for the first time reports the anisotropic atomic displacement parameters (ADPs) of a natural moganite. Rietveld analysis of synchrotron XRD data determined the crystal structure of moganite with the space group I2/a. The refined unit-cell parameters are a = 8.7363(8), b = 4.8688(5), c = 10.7203(9) Å, and β = 90.212(4)°. The ADPs of Si and O in moganite were obtained from X-ray and neutron PDF analyses. The shapes and orientations of the anisotropic ellipsoids determined from X-ray and neutron measurements are similar. The anisotropic ellipsoids for O extend along planes perpendicular to the Si-Si axis of corner-sharing SiO4 tetrahedra, suggesting precession-like movement. Neutron PDF result confirms the occurrence of OH over some of the tetrahedral sites. We postulate that moganite nanomineral is stable with respect to quartz in hypersaline water. The ADPs of moganite show a similar trend as those of quartz determined by single-crystal XRD. In short, the combined methods can provide high-quality structural parameters of moganite nanomineral, including its ADPs and extra OH position at the surface. This approach can be used as an alternative means for solving the structures of crystals that are not large enough for single-crystal XRD measurements, such as fine-grained and nanocrystalline minerals formed in various geological environments.

58 GEOSCIENCES↗
DOE OSTI2022

Description for N = 126 Isotones 210 Po and 212 Rn with Particle-Hole Excited Nucleon-Pair Approximation and Realistic Effective Interaction

In this paper, we study yrast states of two N=126 isotones 210 Po and 212 Rn using the nucleon-pair approximation with particle–hole excitations and using a low-momentum interaction V low–k renormalized from the free CD-Bonn NN potential. An overall good agreement with experimental level structures, B(E2)s, and B(E3)s, is achieved. We also calculate the probabilities of neutron particle–hole excitations in these yrast states, with a focus on negative-parity states, which reflect the roles played by the neutron negative-parity configurations of one-particle-one-hole excitations across the N=126 shell gap and the negative-parity configurations of valence proton particles involving the 0i 13/2 orbit. The N=126 shell gap is discussed in terms of energies of neutron one-particle-one-hole excitations.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Surfactant-free syntheses and pair distribution function analysis of osmium nanoparticles

A surfactant-free synthesis of precious metal nanoparticles (NPs) performed in alkaline low-boiling-point solvents has been recently reported. Monoalcohols are here investigated as solvents and reducing agents to obtain colloidal Os nanoparticles by using low-temperature (<100 °C) surfactant-free syntheses. The effect of the precursor (OsCl 3 or H 2 OsCl 6 ), precursor concentration (up to 100 mM), solvent (methanol or ethanol), presence or absence of a base (NaOH), and addition of water (0 to 100 vol %) on the resulting nanomaterials is discussed. It is found that no base is required to obtain Os nanoparticles as opposed to the case of Pt or Ir NPs. The robustness of the synthesis for a precursor concentration up to 100 mM allows for the performance of X-ray total scattering with pair distribution function (PDF) analysis, which shows that 1–2 nm hexagonal close packed (hcp) NPs are formed from chain-like [OsO x Cl y ] complexes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

The X-shaped Radio Galaxy J0725+5835 is Associated with an AGN Pair

X-shaped radio galaxies (XRGs) are those that exhibit two pairs of unaligned radio lobes (main radio lobes and wings). One of the promising models for the peculiar morphology is jet reorientation. To clarify this, we conducted a 5 GHz observation with the European VLBI Network (EVN) of XRG J0725+5835, which resembles the archetypal binary active galactic nuclei (AGNs) 0402+379 in radio morphology, but it is larger in angular size. In our observation, two milliarcsecond-scale radio components with nonthermal radio emission are detected. Each of them coincides with an optical counterpart with similar photometric redshift and (optical and infrared) magnitude, corresponding to dual active nuclei. Furthermore, with the improved Very Large Array (VLA) images, we find a bridge between the two radio cores and a jet bending in the region surrounding the companion galaxy. This further supports the interplay between the main and companion galaxies. In addition, we also report the discovery of an arcsecond-scale jet in the companion. Given the projected separation of ~100 kpc between the main and companion galaxies, XRG J0725+5835 is likely associated with a dual jetted-AGN system. In both EVN and VLA observations, we find signatures that the jet is changing its direction, which is likely responsible for the X-shaped morphology. For the origin of jet reorientation, several scenarios are discussed.

79 ASTRONOMY AND ASTROPHYSICS↗