Comparative study of free-volume changes in light-cured (dimeth)acrylate-type dental resin composites affected to artificial aging in dry-air and water-immersed mode

Abstract

This research is intended to compare degradation processes in light-cured (dimeth)acrylate-type polymer/filler dental composites affected to aging in dry-air and water-immersed mode. The positron annihilation lifetime (PAL) spectroscopy has been employed to study changes in atomic-deficient structure in these composites under aging. Under light-curing polymerization initiating crosslinking of monomer chains, fragmentation of free-volume holes in resin matrix dominates over enhanced fraction of trapped positrons, since filler–particles assemblies get to be more tightly covered by surrounding polymer causing disappearing of interfacial voids at the filler–polymer surface. Therefore, the PAL spectra-transforming trend in light-cured composites obeys inverse positron-to-Ps trapping conversion. In contrast, the PAL spectra-transforming trend in these restoratives under aging obeys direct Ps-to-positron trapping conversion. After dry-air aging, the observed changes in the density of annihilation sites are ascribed to a strong agglomeration of Ps-decay holes in polymer sub-system accompanied by weaker agglomeration and appearance of positron traps in filler–polymer sub-system. Under the water aging, the agglomeration of Ps-decaying holes in the polymer sub-system is suppressed due to absorbed water molecules, this effect being slightly revealed at lower polymerization. New positron traps are observed at the filler–polymer interfaces in all light-cured composites. The agglomerated Ps-decay holes in a polymer matrix and positron traps inside filler–particles assemblies and filler–polymer interfaces of artificially aged composites cause their progressive microcracking.