The Structure of Gd<sup>3+</sup>-Doped Li<sub>2</sub>O and K<sub>2</sub>O Containing Aluminosilicate Glasses from Molecular Dynamics Simulations
Understanding the atomic structure of glasses is critical for developing new generations of materials with important technical applications. In particular, the local environment of rare-earth ions and their distribution and clustering is of great relevance for applications of rare earth-containing g...
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| author | Mohamed Zekri Andreas Herrmann Andreas Erlebach Kamel Damak Christian Rüssel Marek Sierka Ramzi Maâlej |
| author_facet | Mohamed Zekri Andreas Herrmann Andreas Erlebach Kamel Damak Christian Rüssel Marek Sierka Ramzi Maâlej |
| author_sort | Mohamed Zekri |
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| description | Understanding the atomic structure of glasses is critical for developing new generations of materials with important technical applications. In particular, the local environment of rare-earth ions and their distribution and clustering is of great relevance for applications of rare earth-containing glasses in photonic devices. In this work, the structure of Gd<sub>2</sub>O<sub>3</sub> doped lithium and potassium aluminosilicate glasses is investigated as a function of their network modifier oxide (NMO–Li<sub>2</sub>O, K<sub>2</sub>O) to aluminum oxide ratio using molecular dynamics simulations. The applied simulation procedure yields a set of configurations, the so-called inherent structures, of the liquid state slightly above the glass transition temperature. The generation of a large set of inherent structures allows a statistical sampling of the medium-range order of the Gd<sup>3+</sup> ions with less computational effort compared to other simulation methods. The resulting medium-range atomic structures of network former and modifier ions are in good agreement with experimental results and simulations of similar glasses. It was found that increasing NMO/Al ratio increases the network modifier coordination number with non-bridging oxygen sites and reduces the overall stability of the network structure. The fraction of non-bridging oxygen sites in the vicinity of Gd<sup>3+</sup> ions increases considerably with decreasing field strength and increasing concentration of the network modifier ions. These correlations could be confirmed even if the simulation results of alkaline earth aluminosilicate glasses are added to the analysis. In addition, the structure predictions generally indicate a low driving force for the clustering of Gd<sup>3+</sup>. Here, network modifier ions of large ionic radii reduce the probability of Gd–O–Gd contacts. |
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| language | English |
| last_indexed | 2024-03-10T10:27:36Z |
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| spelling | doaj.art-a833d0c915644ec39d9bfad59644ed442023-11-21T23:55:48ZengMDPI AGMaterials1996-19442021-06-011412326510.3390/ma14123265The Structure of Gd<sup>3+</sup>-Doped Li<sub>2</sub>O and K<sub>2</sub>O Containing Aluminosilicate Glasses from Molecular Dynamics SimulationsMohamed Zekri0Andreas Herrmann1Andreas Erlebach2Kamel Damak3Christian Rüssel4Marek Sierka5Ramzi Maâlej6Georesources Materials Environment and Global Changes Laboratory (GEOGLOB), Faculty of Sciences of Sfax, Sfax University, Sfax 3018, TunisiaInstitute of Materials Science and Engineering, Ilmenau University of Technology, 98693 Ilmenau, GermanyOtto Schott Institute of Materials Research, Friedrich Schiller University Jena, 07743 Jena, GermanyGeoresources Materials Environment and Global Changes Laboratory (GEOGLOB), Faculty of Sciences of Sfax, Sfax University, Sfax 3018, TunisiaOtto Schott Institute of Materials Research, Friedrich Schiller University Jena, 07743 Jena, GermanyOtto Schott Institute of Materials Research, Friedrich Schiller University Jena, 07743 Jena, GermanyGeoresources Materials Environment and Global Changes Laboratory (GEOGLOB), Faculty of Sciences of Sfax, Sfax University, Sfax 3018, TunisiaUnderstanding the atomic structure of glasses is critical for developing new generations of materials with important technical applications. In particular, the local environment of rare-earth ions and their distribution and clustering is of great relevance for applications of rare earth-containing glasses in photonic devices. In this work, the structure of Gd<sub>2</sub>O<sub>3</sub> doped lithium and potassium aluminosilicate glasses is investigated as a function of their network modifier oxide (NMO–Li<sub>2</sub>O, K<sub>2</sub>O) to aluminum oxide ratio using molecular dynamics simulations. The applied simulation procedure yields a set of configurations, the so-called inherent structures, of the liquid state slightly above the glass transition temperature. The generation of a large set of inherent structures allows a statistical sampling of the medium-range order of the Gd<sup>3+</sup> ions with less computational effort compared to other simulation methods. The resulting medium-range atomic structures of network former and modifier ions are in good agreement with experimental results and simulations of similar glasses. It was found that increasing NMO/Al ratio increases the network modifier coordination number with non-bridging oxygen sites and reduces the overall stability of the network structure. The fraction of non-bridging oxygen sites in the vicinity of Gd<sup>3+</sup> ions increases considerably with decreasing field strength and increasing concentration of the network modifier ions. These correlations could be confirmed even if the simulation results of alkaline earth aluminosilicate glasses are added to the analysis. In addition, the structure predictions generally indicate a low driving force for the clustering of Gd<sup>3+</sup>. Here, network modifier ions of large ionic radii reduce the probability of Gd–O–Gd contacts.https://www.mdpi.com/1996-1944/14/12/3265glassaluminosilicaterare earthgadoliniumatomistic simulationsglass structure |
| spellingShingle | Mohamed Zekri Andreas Herrmann Andreas Erlebach Kamel Damak Christian Rüssel Marek Sierka Ramzi Maâlej The Structure of Gd<sup>3+</sup>-Doped Li<sub>2</sub>O and K<sub>2</sub>O Containing Aluminosilicate Glasses from Molecular Dynamics Simulations Materials glass aluminosilicate rare earth gadolinium atomistic simulations glass structure |
| title | The Structure of Gd<sup>3+</sup>-Doped Li<sub>2</sub>O and K<sub>2</sub>O Containing Aluminosilicate Glasses from Molecular Dynamics Simulations |
| title_full | The Structure of Gd<sup>3+</sup>-Doped Li<sub>2</sub>O and K<sub>2</sub>O Containing Aluminosilicate Glasses from Molecular Dynamics Simulations |
| title_fullStr | The Structure of Gd<sup>3+</sup>-Doped Li<sub>2</sub>O and K<sub>2</sub>O Containing Aluminosilicate Glasses from Molecular Dynamics Simulations |
| title_full_unstemmed | The Structure of Gd<sup>3+</sup>-Doped Li<sub>2</sub>O and K<sub>2</sub>O Containing Aluminosilicate Glasses from Molecular Dynamics Simulations |
| title_short | The Structure of Gd<sup>3+</sup>-Doped Li<sub>2</sub>O and K<sub>2</sub>O Containing Aluminosilicate Glasses from Molecular Dynamics Simulations |
| title_sort | structure of gd sup 3 sup doped li sub 2 sub o and k sub 2 sub o containing aluminosilicate glasses from molecular dynamics simulations |
| topic | glass aluminosilicate rare earth gadolinium atomistic simulations glass structure |
| url | https://www.mdpi.com/1996-1944/14/12/3265 |
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