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Probing Compositional Order in Atomic Columns: STEM Simulations Beyond the Virtual Crystal Approximation.

Douglas A Blom1, Thomas Vogt2

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Microscopy and Microanalysis : the Official Journal of Microscopy Society of America, Microbeam Analysis Society, Microscopical Society of Canada
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PubMed
Summary
This summary is machine-generated.

This study uses advanced simulations to analyze compositional disorder in Mo,V-oxide bronze. Findings reveal discrepancies with the virtual crystal approximation, highlighting the importance of atomic arrangements in HAADF-STEM imaging.

Keywords:
HAADF-STEM imagingMo,V-bronzecompositional disorderinstrumental and sample-based noisemultislice frozen-phonon simulationsvirtual crystal approximation

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Area of Science:

  • Materials Science
  • Computational Materials Science
  • Solid-State Chemistry

Background:

  • Compositional disorder in complex oxides impacts material properties.
  • The virtual crystal approximation (VCA) is a common but potentially inaccurate method for modeling disorder.
  • Experimental techniques like HAADF-STEM are sensitive to atomic arrangements.

Purpose of the Study:

  • To investigate compositional disorder in Mo,V-oxide bronze using advanced computational methods.
  • To compare simulation results with experimental data and identify limitations of the VCA.
  • To determine the influence of atomic ordering on high-angle annular dark-field (HAADF) imaging.

Main Methods:

  • Multislice frozen-phonon calculations utilizing parallel computing.
  • Modeling compositional disorder in metal-oxygen atomic columns.
  • Analysis of high-angle annular dark-field (HAADF) imaging simulations and experimental data.

Main Results:

  • The virtual crystal approximation underestimates V content in Mo,V-oxide bronze compared to simulations considering cation ordering.
  • Discrepancies between VCA and simulations exceed the variability caused by different atomic configurations.
  • HAADF-STEM imaging can distinguish between ordered and random atomic arrangements along columns.
  • Simulated intensity variations qualitatively match experimental HAADF-STEM data for Mo,V-oxide bronze.

Conclusions:

  • The VCA is insufficient for accurately modeling compositional disorder in this system.
  • Atomic ordering significantly influences HAADF-STEM image intensities.
  • A limited number of random configurations can effectively represent intensity variations, improving simulation accuracy.