The impact of nitridation on open volumes in thin HfSiOx films fabricated on Si substrates by atomic layer deposition was studied using monoenergetic positron beams. For HfSiOx, positrons were found to annihilate from the trapped state due to open volumes which exist intrinsically in an amorphous structure. After plasma nitridation, the size of open volumes decreased at a nitrogen concentration of about 20 at. %. An expansion of open volumes, however, was observed after postnitridation annealing (PNA) (1050°C, 5 s). We found that the size of open volumes increased with increasing nitrogen concentration in HfSiOx. The change in the size of open volumes was attributed to the trapping of nitrogen by open volumes, and an incorporation of nitrogen into the amorphous matrix of HfSiOx during PNA. We also examined the role of nitrogen in HfSiOx using x-ray photoelectron spectroscopy and first principles calculations.
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