Browse
Submit Data
Databases
API
Help

Dataset Information

0 Views

0 Connections

0 Citations

0 Reanalyses

0 Downloads

Omics score: 0

Extracting interface correlations from the pair distribution function of composite materials.

ABSTRACT: Using a non-negative matrix factorisation (NMF) approach, we show how the pair distribution function (PDF) of complex mixtures can be deconvolved into the contributions from the individual phase components and also the interface between phases. Our focus is on the model system Fe∥Fe₃O₄. We establish proof-of-concept using idealised PDF data generated from established theory-driven models of the Fe∥Fe₃O₄ interface. Using X-ray total scattering measurements for corroded Fe samples, and employing our newly-developed NMF analysis, we extract the experimental interface PDF ('iPDF') for this same system. We find excellent agreement between theory and experiment. The implications of our results in the broader context of interface characterisation for complex functional materials are discussed.

SUBMITTER: Geddes HS

PROVIDER: S-EPMC8359142 | biostudies-literature | 2021 Aug

REPOSITORIES: biostudies-literature

ACCESS DATA

Json Xml

Publications

Extracting interface correlations from the pair distribution function of composite materials.

Geddes Harry S HS Hutchinson Henry D HD Ha Alex R AR Funnell Nicholas P NP Goodwin Andrew L AL

Nanoscale 20210730 31

Using a non-negative matrix factorisation (NMF) approach, we show how the pair distribution function (PDF) of complex mixtures can be deconvolved into the contributions from the individual phase components and also the interface between phases. Our focus is on the model system Fe∥Fe3O4. We establish proof-of-concept using idealised PDF data generated from established theory-driven models of the Fe∥Fe3O4 interface. Using X-ray total scattering measureme ...[more]

PMID: 34477729

Similar Datasets

Structural Analysis of Molecular Materials Using the Pair Distribution Function.

Project description:This is a review of atomic pair distribution function (PDF) analysis as applied to the study of molecular materials. The PDF method is a powerful approach to study short- and intermediate-range order in materials on the nanoscale. It may be obtained from total scattering measurements using X-rays, neutrons, or electrons, and it provides structural details when defects, disorder, or structural ambiguities obscure their elucidation directly in reciprocal space. While its uses in the study of inorganic crystals, glasses, and nanomaterials have been recently highlighted, significant progress has also been made in its application to molecular materials such as carbons, pharmaceuticals, polymers, liquids, coordination compounds, composites, and more. Here, an overview of applications toward a wide variety of molecular compounds (organic and inorganic) and systems with molecular components is presented. We then present pedagogical descriptions and tips for further implementation. Successful utilization of the method requires an interdisciplinary consolidation of material preparation, high quality scattering experimentation, data processing, model formulation, and attentive scrutiny of the results. It is hoped that this article will provide a useful reference to practitioners for PDF applications in a wide realm of molecular sciences, and help new practitioners to get started with this technique.

| S-EPMC8759070 | biostudies-literature

EDP2PDF: a computer program for extracting a pair distribution function from an electron diffraction pattern for the structural analysis of materials.

Project description:Pair distribution function (PDF) analysis is a powerful technique to understand atomic scale structure in materials science. Unlike X-ray diffraction (XRD)-based PDF analysis, the PDF calculated from electron diffraction patterns (EDPs) using transmission electron microscopy can provide structural information from specific locations with high spatial resolution. The present work describes a new software tool for both periodic and amorphous structures that addresses several practical challenges in calculating the PDF from EDPs. The key features of this program include accurate background subtraction using a nonlinear iterative peak-clipping algorithm and automatic conversion of various types of diffraction intensity profiles into a PDF without requiring external software. The present study also evaluates the effect of background subtraction and the elliptical distortion of EDPs on PDF profiles. The EDP2PDF software is offered as a reliable tool to analyse the atomic structure of crystalline and non-crystalline materials.

| S-EPMC10241047 | biostudies-literature

Time-resolved pair distribution function analysis of disordered materials on beamlines BL04B2 and BL08W at SPring-8.

Project description:A dedicated apparatus has been developed for studying structural changes in amorphous and disordered crystalline materials substantially in real time. The apparatus, which can be set up on beamlines BL04B2 and BL08W at SPring-8, mainly consists of a large two-dimensional flat-panel detector and high-energy X-rays, enabling total scattering measurements to be carried out for time-resolved pair distribution function (PDF) analysis in the temperature range from room temperature to 873 K at pressures of up to 20 bar. For successful time-resolved analysis, a newly developed program was used that can monitor and process two-dimensional image data simultaneously with the data collection. The use of time-resolved hardware and software is of great importance for obtaining a detailed understanding of the structural changes in disordered materials, as exemplified by the results of commissioned measurements carried out on both beamlines. Benchmark results obtained using amorphous silica and demonstration results for the observation of sulfide glass crystallization upon annealing are introduced.

| S-EPMC6225740 | biostudies-literature

A Comparative Study of Experimental Configurations in Synchrotron Pair Distribution Function.

Project description:The identification and quantification of amorphous components and nanocrystalline phases with very small crystal sizes, smaller than ~3 nm, within samples containing crystalline phases is very challenging. However, this is important as there are several types of systems that contain these matrices: building materials, glass-ceramics, some alloys, etc. The total scattering synchrotron pair distribution function (PDF) can be used to characterize the local atomic order of the nanocrystalline components and to carry out quantitative analyses in complex mixtures. Although the resolution in momentum transfer space has been widely discussed, the resolution in the interatomic distance space has not been discussed to the best of our knowledge. Here, we report synchrotron PDF data collected at three beamlines in different experimental configurations and X-ray detectors. We not only discuss the effect of the resolution in Q-space, Qmax ins of the recorded data and Qmax of the processed data, but we also discuss the resolution in the interatomic distance (real) space. A thorough study of single-phase crystalline nickel used as standard was carried out. Then, selected cement-related samples including anhydrous tricalcium and dicalcium silicates, and pastes derived from the hydration of tricalcium silicate and ye'elimite with bassanite were analyzed.

| S-EPMC6515447 | biostudies-literature

Zr4+ solution structures from pair distribution function analysis.

Project description:The structures of metal ions in solution constitute essential information for obtaining chemical insight spanning from catalytic reaction mechanisms to formation of functional nanomaterials. Here, we explore Zr4+ solution structures using X-ray pair distribution function (PDF) analysis across pH (0-14), concentrations (0.1-1.5 M), solvents (water, methanol, ethanol, acetonitrile) and metal sources (ZrCl4, ZrOCl2·8H2O, ZrO(NO3)2·xH2O). In water, [Zr4(OH)8(OH2)16]8+-tetramers are predominant, while non-aqueous solvents contain monomeric complexes. The PDF analysis also reveals second sphere coordination of chloride counter ions to the aqueous tetramers. The results are reproducible across data measured at three different beamlines at the PETRA-III and MAX IV synchrotron light sources.

| S-EPMC9645415 | biostudies-literature

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

Project description: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 (OsCl3 or H2OsCl6), 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.

| S-EPMC8895034 | biostudies-literature

Nonlinear backbone torsional pair correlations in proteins.

Project description:Protein allostery requires dynamical structural correlations. Physical origin of which, however, remain elusive despite intensive studies during last two and half decades. Based on analysis of molecular dynamics (MD) simulation trajectories for ten proteins with different sizes and folds, we found that nonlinear backbone torsional pair (BTP) correlations, which are mainly spatially long-ranged and are dominantly executed by loop residues, exist extensively in most analyzed proteins. Examination of torsional motion for correlated BTPs suggested that such nonlinear correlations are mainly associated aharmonic torsional state transitions and in some cases strongly anisotropic local torsional motion of participating torsions, and occur on widely different and relatively longer time scales. In contrast, correlations between backbone torsions in stable α helices and β strands are mainly linear and spatially short-ranged, and are more likely to associate with harmonic local torsional motion. Further analysis revealed that the direct cause of nonlinear contributions are heterogeneous linear correlations. These findings implicate a general search strategy for novel allosteric modulation sites of protein activities.

| S-EPMC5052647 | biostudies-literature

Operando pair distribution function analysis of nanocrystalline functional materials: the case of TiO2-bronze nanocrystals in Li-ion battery electrodes.

Project description:Structural modelling of operando pair distribution function (PDF) data of complex functional materials can be highly challenging. To aid the understanding of complex operando PDF data, this article demonstrates a toolbox for PDF analysis. The tools include denoising using principal component analysis together with the structureMining, similarityMapping and nmfMapping apps available through the online service 'PDF in the cloud' (PDFitc, https://pdfitc.org/). The toolbox is used for both ex situ and operando PDF data for 3 nm TiO2-bronze nanocrystals, which function as the active electrode material in a Li-ion battery. The tools enable structural modelling of the ex situ and operando PDF data, revealing two pristine TiO2 phases (bronze and anatase) and two lithiated Li x TiO2 phases (lithiated versions of bronze and anatase), and the phase evolution during galvanostatic cycling is characterized.

| S-EPMC11299615 | biostudies-literature

Direct determination of amorphous number density from the reduced pair distribution function.

Project description:The inference of amorphous bulk density, while straightforward for nonporous, soluble materials, may present a formidable challenge in some of the most important classes of industrial applications, involving melts, porous solids, and non-soluble organic pharmaceuticals, with varied implications depending on the material's level of technological interest. Within nanotechnology and the life sciences in particular, accurate determination of amorphous true density is a frequent requirement and a regular puzzle, when, e.g., neither the Archimedean principle nor gas pycnometry may be applied, the former being only applicable to insoluble compounds, while the latter yielding skeletal density - an overestimate of true density to the extent of blind pores - and its efficiency is affected by the choice of the gas medium. In these cases, it is feasible to infer amorphous density from diffraction experiments through the use of the reduced Pair Distribution Function (PDF). Although an estimate of crystalline density has been known to be possible via the PDF shape, here we outline a new method extending this facility to include the estimation of amorphous density. •Amorphous density may be inferred from the position of a local minimum of the reduced PDF profile, the latter extracted via a Fourier transformation of collected diffraction intensity.•The PDF minimum is located within the PDF range bounded by rmin = 2π/Qmax and the position of the first coordination peak, where Qmax is the maximum length of the scattering vector achieved in the diffraction experiment.•Amorphous density is calculated as the ratio of the value of the reduced PDF at the local minimum, divided by the term 4πr, where r is the real space coordinate of the local minimum.

| S-EPMC6446046 | biostudies-literature

Interface Engineering of Styrenic Polymer Grafted Porous Micro-Silicon/Polyaniline Composite for Enhanced Lithium Storage Anode Materials

Project description: Not available

| S-EPMC11679390 | biostudies-literature