Pair distribution function analysis of discrete nanomaterials in PDFgui

Chen, Zhihengyu; Beauvais, Michelle L.; Chapman, Karena W.

doi:10.1107/s1600576723000237

Pair distribution function analysis of discrete nanomaterials in PDFgui

Journal Article · Fri Feb 24 00:00:00 EST 2023 · Journal of Applied Crystallography (Online)

DOI:https://doi.org/10.1107/s1600576723000237· OSTI ID:2404489

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Stony Brook University, NY (United States); University of Chicago
Stony Brook University, NY (United States)

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.

View Accepted Manuscript (DOE)

Research Organization:: University of Chicago, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: SC0012702; SC0012704; SC0019212; SC0023383

OSTI ID:: 2404489

Journal Information:: Journal of Applied Crystallography (Online), Journal Name: Journal of Applied Crystallography (Online) Journal Issue: 2 Vol. 56; ISSN 1600-5767

Publisher:: International Union of CrystallographyCopyright Statement

Country of Publication:: United States

Language:: English

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