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The results of measurements of X‐ray photoelectron spectra (XPS) of a‐SiO 2  host material after pulsed implantation with [Mn + ] and [Co + , Mn + ] ions as well as DFT‐calculations are presented. The low‐energy shift is found in XPS Si 2 p  and O 1 s  core‐levels of single [Mn + ] and dual [Co + , Mn + ] pulsed ion‐implanted a‐SiO 2  ( E  = 30 keV,  D  = 2×10 17  cm −2 ) with respect to those of untreated a‐SiO 2 . Similar changes are found in XPS Si 2 p  and O 1 s  of stishovite compared to those of quartz. This means that the pulsed ion implantation induces the local high pressure effect that leads to the appearance of SiO 6 ‐structural units in a‐SiO 2  host, forming “stishovite‐like” local atomic structure. This process can be described within an electronic bonding transition from the fourfold “quartz‐like” to sixfold “stishovite‐like” high‐pressure phase in the SiO 2  host matrix. It is found that such octahedral conversion depends on the fluence and starts with doses higher than  D  = 3×10 16  cm −2 .

Octahedral conversion of a‐SiO 2 host matrix by pulsed ion implantation