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Although molecular dynamics (MD) simulation is a powerful tool for investigating the atomic-scale structures of complex materials, several challenges limit their reliable and accurate application to multi-component glass systems. The available force fields (FFs) that can treat many elements in a multi-component glass are limited, and even if such a FF exists, its accuracy is suspicious due to the large variety and complexity of chemical environments in these materials. First-principles calculations based on the density functional theory (DFT) are reliable, but prohibitively expensive with conventional methods.
In this study, we use large-scale DFT techniques and demonstrate that it is possible to perform efficient and accurate DFT calculations of multi-component glass systems, such as (SiO$_2$)$_{0.70}$(Al$_2$O$_3$)$_{0.13}$($X$O)$_{0.17}$ ($X$ = Mg, Ca, Sr, Ba), containing about 1,000--5,000 atoms.
From the results of large-scale DFT calculations, we evaluate the accuracy of some classical FFs,
and show that the accuracy for non-bridging oxygen atoms is very low especially when the Si--O distance is short. Large differences in the distribution of Si--O--Si angles observed in the FF-MD and DFT-MD simulations
and the unique electronic structure in the case of $X$=Mg are also discussed.

Rights:

• Creative Commons BY Attribution 4.0 International
  

Keyword: Multi-component glass, First-principles calculations, Large-scale DFT, Classical force fields, Molecular dynamics simulations

Date published: 2023-11-25

Publisher: Elsevier BV

Journal:

• Journal of Non-Crystalline Solids (ISSN: 00223093) vol. 625 p. 122714- 122714

Funding:

• MEXT, Japan and JSPS Grant-in-Aid JP20H05883 (Trans- formative Research Areas (A) ‘‘Hyper-Ordered Structures Science’’)
• JASRI 2019B2007 (synchrotron radiation experiments)

Manuscript type: Publisher's version (Version of record)

MDR DOI:

First published URL: https://doi.org/10.1016/j.jnoncrysol.2023.122714

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Updated at: 2024-03-05 16:30:21 +0900

Published on MDR: 2024-03-05 16:30:22 +0900