L. Zhang et al., ROLE OF RADIOLYTIC OXYGEN IN THE X-RAY-PRODUCTION AND THERMAL ANNEALING OF DEFECTS IN HIGH-PURITY AMORPHOUS SIO2, Physical review. B, Condensed matter, 53(11), 1996, pp. 7182-7189
Direct experimental evidence for the presence and x-ray dose dependenc
e of radiolytically displaced oxygen in high-purity, oxygen-deficient
a-SiO2 is presented. Anneal-interrupted x-irradiation and electron spi
n resonance measurements were used to investigate the x-ray dose depen
dence of the radiation response of two types of low-OH a-SiO2, i.e., o
xygen-excess and oxygen-deficient materials. The production and therma
l annealing of paramagnetic defects in these two materials were compar
ed to explore the role played by dissolved and radiolytically displace
d oxygen in these processes. The multiple, reversible interconversions
of E' centers and peroxy radicals proved to be very sensitive to the
presence of free oxygen in the a-SiO2 network. Such interconversions a
re very probable in the oxygen-excess material due to the presence of
dissolved oxygen. It follows that such interconversions an not expecte
d in the oxygen-deficient material, at least at low dose, in agreement
with experimental data. However, our results show that such interconv
ersions take place above a certain threshold dose in oxygen-deficient
material. In fact, we observed peroxy radicals in oxygen-deficient mat
erial. Their production is attributed to the presence of radiolyticall
y displaced oxygen in this material. A simple physical model is presen
ted to explain the results. The model involves the random creation of
displaced oxygen atoms which undergo elastically driven recombination
into oxygen molecules. It is these molecules which participate in the
interconversions in the oxygen-deficient material. A threshold is obse
rved because the recombination does not occur unless the distance betw
een the oxygen atoms is less than some characteristic length, i.e., a
correlation radius of an elastically coherent nanoregion in the amorph
ous network. The experimental results and the model imply a universal
radiation response at high dose when the density of radiolytically dis
placed oxygen exceeds that of any precursors.