Novel Oxygen-Deficient Centers and Other Intrinsic Defects in Amorphous SiO2: Quantum Molecular Dynamics Simulations

Vladimir B. Sulimov; Danil C. Kutov; Alexey V. Sulimov; Fedor V. Grigoriev; Alexander A. Tikhonravov

doi:10.14529/jsfi250407

Authors

Vladimir B. Sulimov Research Computing Center of Lomonosov Moscow State University, Moscow, Russian Federation https://orcid.org/0000-0002-7102-6107
Danil C. Kutov Research Computing Center of Lomonosov Moscow State University, Moscow, Russian Federation https://orcid.org/0000-0002-4777-6522
Alexey V. Sulimov Research Computing Center of Lomonosov Moscow State University, Moscow, Russian Federation https://orcid.org/0000-0002-8767-642X
Fedor V. Grigoriev Research Computing Center of Lomonosov Moscow State University, Moscow, Russian Federation https://orcid.org/0000-0001-6893-3008
Alexander A. Tikhonravov Research Computing Center of Lomonosov Moscow State University, Moscow, Russian Federation https://orcid.org/0000-0003-4240-7709

DOI:

https://doi.org/10.14529/jsfi250407

Keywords:

quantum molecular dynamics, amorphous SiO2, point defects, oxygen deficiency, oxygen vacancy, ODC

Abstract

The formation of stoichiometric and oxygen-deficient amorphous states of a-SiO₂from a corresponding crystal was simulated using the melting-quenching procedure. To simulate the entire process, quantum molecular dynamics implemented in the VASP program and supercells containing 64 Si atoms and 128 O atoms were used. This size allows modeling the formation of rings with a small number of Si–O–Si bridges. At given heating and cooling rates of 0.5 K/fs, the transformation of the crystal’s atomic network into a disordered structure was studied depending on the melt stabilization temperature. It is shown that despite the strong change in the topology of the atomic network in a-SiO₂compared to the crystal, the bulk of the atoms constitute a continuous network of SiO₄tetrahedra linked by oxygen vertices. Local disturbances of this arrangement of atoms are intrinsic point defects of SiO₂, which are given special attention. It has been shown that most of the defects present in oxygen-deficient states are also present in stoichiometric states of a-SiO₂. Along with the known intrinsic defects of SiO₂, new defects were also identified, including those associated with oxygen deficiency. It is shown that for two generally accepted models of oxygen-deficient centers (ODCs) in a-SiO₂, the energy of formation of an oxygen vacancy is significantly lower than the energy of formation of a twofold coordinated silicon atom. The point defects of a-SiO₂identified in this work create a foundation for the interpretation of experimental data on the radiation resistance of optical fibers, the effects of high-power laser radiation on optical coatings, and in microelectronics, where insulating layers based on a-SiO₂are used.

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