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Title: Pair distribution function analysis applied to decahedral gold nanoparticles

Abstract

The five-fold symmetry of face-centered cubic (fcc) derived nanoparticles is inconsistent with the translational symmetry of a Bravais lattice and generally explained by multiple twinning of a tetrahedral subunit about a (joint) symmetry axis, with or without structural modification to the fcc motif. Unlike in bulk materials, five-fold twinning in cubic nanoparticles is common and strongly affects their structural, chemical, and electronic properties. To test and verify theoretical approaches, it is therefore pertinent that the local structural features of such materials can be fully characterized. The small size of nanoparticles severely limits the application of traditional analysis techniques, such as Bragg diffraction. A complete description of the atomic arrangement in nanoparticles therefore requires a departure from the concept of translational symmetry, and prevents fully evaluating all the structural features experimentally. We describe how recent advances in instrumentation, together with the increasing power of computing, are shaping the development of alternative analysis methods of scattering data for nanostructures. We present the application of Debye scattering and pair distribution function (PDF) analysis towards modeling of the total scattering data for the example of decahedral gold nanoparticles. PDF measurements provide a statistical description of the pair correlations of atoms within a material, allowingmore » one to evaluate the probability of finding two atoms within a given distance. We explored the sensitivity of existing synchrotron x-ray PDF instruments for distinguishing four different simple models for our gold nanoparticles: a multiply twinned fcc decahedron with either a single gap or multiple distributed gaps, a relaxed body-centered orthorhombic (bco) decahedron, and a hybrid decahedron. The data simulations of the models were then compared with experimental data from synchrotron x-ray total scattering. We present our experimentally derived atomistic models of the gold nanoparticles, with surprising results and a perspective on remaining challenges. Lastly, our findings provide evidence for the suitability of PDF analysis in the characterization of other nanosized particles that may have commercial applications.« less

Authors:
 [1];  [1];  [2];  [2]; ORCiD logo [2];  [1];  [3];  [1];  [4];  [3]
  1. New Mexico State Univ., Las Cruces, NM (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  3. Univ. of California - San Diego, La Jolla, CA (United States)
  4. New Mexico State Univ., Las Cruces, NM (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1510593
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Physica Scripta
Additional Journal Information:
Journal Volume: 92; Journal Issue: 11; Journal ID: ISSN 0031-8949
Publisher:
IOP Publishing
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; decahedral nanoparticles; pair-distribution function analysis; CVD growth; Bragg diffraction

Citation Formats

Nakotte, H., Silkwood, C., Page, K., Wang, H-W, Olds, D., Kiefer, B., Manna, S., Karpov, D., Fohtung, E., and Fullerton, E. E. Pair distribution function analysis applied to decahedral gold nanoparticles. United States: N. p., 2017. Web. doi:10.1088/1402-4896/aa8afd.
Nakotte, H., Silkwood, C., Page, K., Wang, H-W, Olds, D., Kiefer, B., Manna, S., Karpov, D., Fohtung, E., & Fullerton, E. E. Pair distribution function analysis applied to decahedral gold nanoparticles. United States. doi:10.1088/1402-4896/aa8afd.
Nakotte, H., Silkwood, C., Page, K., Wang, H-W, Olds, D., Kiefer, B., Manna, S., Karpov, D., Fohtung, E., and Fullerton, E. E. Mon . "Pair distribution function analysis applied to decahedral gold nanoparticles". United States. doi:10.1088/1402-4896/aa8afd. https://www.osti.gov/servlets/purl/1510593.
@article{osti_1510593,
title = {Pair distribution function analysis applied to decahedral gold nanoparticles},
author = {Nakotte, H. and Silkwood, C. and Page, K. and Wang, H-W and Olds, D. and Kiefer, B. and Manna, S. and Karpov, D. and Fohtung, E. and Fullerton, E. E.},
abstractNote = {The five-fold symmetry of face-centered cubic (fcc) derived nanoparticles is inconsistent with the translational symmetry of a Bravais lattice and generally explained by multiple twinning of a tetrahedral subunit about a (joint) symmetry axis, with or without structural modification to the fcc motif. Unlike in bulk materials, five-fold twinning in cubic nanoparticles is common and strongly affects their structural, chemical, and electronic properties. To test and verify theoretical approaches, it is therefore pertinent that the local structural features of such materials can be fully characterized. The small size of nanoparticles severely limits the application of traditional analysis techniques, such as Bragg diffraction. A complete description of the atomic arrangement in nanoparticles therefore requires a departure from the concept of translational symmetry, and prevents fully evaluating all the structural features experimentally. We describe how recent advances in instrumentation, together with the increasing power of computing, are shaping the development of alternative analysis methods of scattering data for nanostructures. We present the application of Debye scattering and pair distribution function (PDF) analysis towards modeling of the total scattering data for the example of decahedral gold nanoparticles. PDF measurements provide a statistical description of the pair correlations of atoms within a material, allowing one to evaluate the probability of finding two atoms within a given distance. We explored the sensitivity of existing synchrotron x-ray PDF instruments for distinguishing four different simple models for our gold nanoparticles: a multiply twinned fcc decahedron with either a single gap or multiple distributed gaps, a relaxed body-centered orthorhombic (bco) decahedron, and a hybrid decahedron. The data simulations of the models were then compared with experimental data from synchrotron x-ray total scattering. We present our experimentally derived atomistic models of the gold nanoparticles, with surprising results and a perspective on remaining challenges. Lastly, our findings provide evidence for the suitability of PDF analysis in the characterization of other nanosized particles that may have commercial applications.},
doi = {10.1088/1402-4896/aa8afd},
journal = {Physica Scripta},
number = 11,
volume = 92,
place = {United States},
year = {2017},
month = {10}
}

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