Atomic and Electronic Structure in MgO–SiO2

Shuseki, Yuta; Kohara, Shinji; Kaneko, Tomoaki; Sodeyama, Keitaro; Onodera, Yohei; Koyama, Chihiro; Masuno, Atsunobu; Sasaki, Shunta; Hatano, Shohei; Shiga, Motoki; Obayashi, Ippei; Hiraoka, Yasuaki; Okada, Junpei T.; Mizuno, Akitoshi; Watanabe, Yuki; Nakata, Yui; Ohara, Koji; Murakami, Motohiko; Tucker, Matthew G.; McDonnell, Marshall T.; Oda, Hirohisa; Ishikawa, Takehiko

doi:10.1021/acs.jpca.3c05561

Title: Atomic and Electronic Structure in MgO–SiO₂

Journal Article · 17 January 2024 · Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory

DOI: https://doi.org/10.1021/acs.jpca.3c05561 · OSTI ID:2438746

^[1];

^[2]; Kaneko, Tomoaki ^[3];

^[2]; Onodera, Yohei ^[2]; Koyama, Chihiro ^[4]; Masuno, Atsunobu ^[1]; Sasaki, Shunta ^[5]; Hatano, Shohei ^[5]; Shiga, Motoki ^[6]; Obayashi, Ippei ^[7]; Hiraoka, Yasuaki ^[8]; Okada, Junpei T. ^[9];

^[10]; Watanabe, Yuki ^[11]; Nakata, Yui ^[11];

^[12]; Murakami, Motohiko ^[13];

^[14];

^[14] more »

Kyoto Univ. (Japan); National Institute for Materials Science (NIMS), Tsukuba (Japan)
National Institute for Materials Science (NIMS), Tsukuba (Japan)
Research Organization for Information Science and Technology (RIST), Tokyo (Japan)
Japan Aerospace Exploration Agency (JAXA), Tsukuba (Japan)
Hirosaki Univ. (Japan)
Tohoku Univ., Sendai (Japan); Institute of Physical and Chemical Research (RIKEN), Tokyo (Japan)
Okayama Univ. (Japan)
Kyoto Univ. (Japan)
Tohoku Univ., Sendai (Japan)
National Institute of Technology (Japan)
Advanced Engineering Services Co., Ltd. (Japan)
Shimane University (Japan)
Eidgenoessische Technische Hochschule (ETH), Zurich (Switzerland)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Understanding disordered structure is difficult due to insufficient information in experimental data. Here, we overcome this issue by using a combination of diffraction and simulation to investigate oxygen packing and network topology in glassy (g-) and liquid (l-) MgO–SiO₂ based on a comparison with the crystalline topology. We find that packing of oxygen atoms in Mg₂SiO₄ is larger than that in MgSiO₃, and that of the glasses is larger than that of the liquids. Moreover, topological analysis suggests that topological similarity between crystalline (c)- and g-(l-) Mg₂SiO₄ is the signature of low glass-forming ability (GFA), and high GFA g-(l-) MgSiO₃ shows a unique glass topology, which is different from c-MgSiO₃. We also find that the lowest unoccupied molecular orbital (LUMO) is a free electron-like state at a void site of magnesium atom arising from decreased oxygen coordination, which is far away from crystalline oxides in which LUMO is occupied by oxygen’s 3s orbital state in g- and l-MgO–SiO₂, suggesting that electronic structure does not play an important role to determine GFA. We finally concluded the GFA of MgO–SiO₂ binary is dominated by the atomic structure in terms of network topology.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 2438746

Journal Information:: Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory, Journal Name: Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory Journal Issue: 4 Vol. 128; ISSN 1089-5639

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
amorphous materials
chemical structure
liquids
oxygen
x-rays

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