Effect of temperature and thermal history on borosilicate glass structure

Frédéric Angeli, Olivier Villain, Sophie Schuller, Thibault Charpentier, Dominique de Ligny, Lena Bressel, and Lothar Wondraczek
Phys. Rev. B 85, 054110 – Published 14 February 2012

Abstract

The influence of the temperature and quenching rate on the structure of a borosilicate glass was studied by high-resolution solid-state 11B, 23Na, 29Si nuclear magnetic resonance (NMR) and high-temperature Raman spectroscopy. Data were obtained for glass in the solid state after annealing and quenching at cooling rates covering four orders of magnitude as well as in the liquid state from Raman experiments and from calorimetry and rheological data. Nuclear magnetic resonance measurements were used to calibrate the Raman spectra in order to quantify the change in boron coordination with temperature. This result can then be used to determine the fictive temperature of the glass directly from the boron coordination. The fictive temperature, heat capacity, and configurational entropy are extracted from calorimetry and viscosity measurements. Changes in the boron coordination account for only 25% of the configurational heat capacity of the liquid. The structural parameters capable of accounting for the remaining quantity are discussed on the basis of structural data, both local (inhomogeneity of the sodium distribution) and medium-range (from NMR parameter distribution). It has thus been shown that, although the B-O-B angular distributions of the boroxol rings (and probably the Si-O-Si distributions) are not affected by temperature, a structural disorder is identified through the angular distributions of the bonds linking borate and silicate groups.

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  • Received 28 September 2011

DOI:https://doi.org/10.1103/PhysRevB.85.054110

©2012 American Physical Society

Authors & Affiliations

Frédéric Angeli1,*, Olivier Villain2, Sophie Schuller3, Thibault Charpentier2, Dominique de Ligny4, Lena Bressel4, and Lothar Wondraczek5

  • 1CEA, DEN, Laboratoire d’étude du Comportement à Long Terme, 30207 Bagnols-sur-Cèze, France
  • 2CEA, IRAMIS, Laboratoire de Structure et Dynamique par Résonance Magnétique, UMR CEA/CNRS 3299, 91191 Gif-sur-Yvette, France
  • 3CEA, DEN, Laboratoire d’étude et Développement des Matrices de Confinement, 30207 Bagnols-sur-Cèze, France
  • 4Université de Lyon, Université Lyon 1, CNRS, UMR5620, Laboratoire de Physico-Chimie des Matériaux Luminescents, F-69622 Villeurbanne, France
  • 5Department of Material Science, Glass and Ceramics-WW3, University of Erlangen-Nuremberg, 91058 Erlangen, Germany

  • *Corresponding author: Dr. Frédéric Angeli, CEA Marcoule, DEN/DTCD/SECM/LCLT, BP 17171, 30207 Bagnols-sur-cze, France; frederic.angeli@cea.fr

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Vol. 85, Iss. 5 — 1 February 2012

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