Structure and properties of densified silica glass: characterizing the order within disorder

Yohei Onodera, Shinji Kohara, Philip S. Salmon, Akihiko Hirata, Norimasa Nishiyama, Suguru Kitani, Anita Zeidler, Motoki Shiga, Atsunobu Masuno, Hiroyuki Inoue, Shuta Tahara, Annalisa Polidori, Henry E. Fischer, Tatsuya Mori, Seiji Kojima, Hitoshi Kawaji, Alexander I. Kolesnikov, Matthew B. Stone, Matthew G. Tucker, Marshall T. McDonnellAlex C. Hannon, Yasuaki Hiraoka, Ippei Obayashi, Takenobu Nakamura, Jaakko Akola, Yasuhiro Fujii, Koji Ohara, Takashi Taniguchi, Osami Sakata

Research output: Contribution to journalArticlepeer-review

Abstract

The broken symmetry in the atomic-scale ordering of glassy versus crystalline solids leads to a daunting challenge to provide suitable metrics for describing the order within disorder, especially on length scales beyond the nearest neighbor that are characterized by rich structural complexity. Here, we address this challenge for silica, a canonical network-forming glass, by using hot versus cold compression to (i) systematically increase the structural ordering after densification and (ii) prepare two glasses with the same high-density but contrasting structures. The structure was measured by high-energy X-ray and neutron diffraction, and atomistic models were generated that reproduce the experimental results. The vibrational and thermodynamic properties of the glasses were probed by using inelastic neutron scattering and calorimetry, respectively. Traditional measures of amorphous structures show relatively subtle changes upon compacting the glass. The method of persistent homology identifies, however, distinct features in the network topology that change as the initially open structure of the glass is collapsed. The results for the same high-density glasses show that the nature of structural disorder does impact the heat capacity and boson peak in the low-frequency dynamical spectra. Densification is discussed in terms of the loss of locally favored tetrahedral structures comprising oxygen-decorated SiSi4 tetrahedra.

Original languageEnglish
Article number85
JournalNPG Asia Materials
Volume12
Issue number1
DOIs
Publication statusPublished - 2020 Dec

ASJC Scopus subject areas

  • Modelling and Simulation
  • Materials Science(all)
  • Condensed Matter Physics

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