First principles study of oxygen vacancy defects in amorphous SiO2

The oxygen vacancy defects of amorphous SiO2 (a-SiO2) in different charge states are investigated by the periodic density functional theory. Five types of the positively charged configurations are obtained including the dimer, forward-oriented, puckered 4×, 5× and back-projected unpuckered configurations. The energy, geometry structure, spin density, Bader charge and Fermi contact are concerned for these systems. These defects can be regarded as the potential microscopic structures for the corresponding centers including Eα′, Eγ′ and Eδ′ in the electron paramagnetic resonance (EPR) experiments. Then, the charge-state transitions of these defects are investigated by intentionally adding one electron to the positively charged systems. For the dimer, puckered 4× and back-projected unpuckered configurations, all of the corresponding neutral species maintain their initial types of geometry structures. For the forward-oriented configurations, the corresponding neutral species transform into the structures of the divalent Si atom. The puckered 5× configurations have the most abundant neutral species: some of them could maintain its style of the puckered 5× configurations, and some collapse to the neutral dimer or forward-oriented configurations. The dimer configurations have the lowest thermodynamic charge-state levels, and the puckered 4× configurations have the highest thermodynamic charge-state levels among the five types of configurations. This work is of benefit to identifying and controlling the oxygen defects in a-SiO2.