Nanostructure of thin amorphous hydrogenated carbon films studied by positron annihilation and photoluminescence

Abstract

We deposited polymer-like a-C:H films using the plasma-enhanced chemical vapor deposition technique and characterized film microstructure by variable-energy positron lifetime spectroscopy, photoluminescence (PL), and UV-visible absorption spectroscopy. It was confirmed that PL occurs from a chromophore in a sp2 cluster as a result of fast recombination of a photoexcited electron-hole pair. Positron annihilation lifetime spectroscopy showed that positronium (Ps) formation takes place via electron-positron recombination in the sp3 matrix. The lifetime of ortho-positronium (o-Ps) in our a-C:H films was similar to that in polyethylene, indicating their polymer-like nature. The relative PL efficiency increased by about an order of magnitude with increasing film band gap from 1.3 to 3.4 eV, which can be related to the decreasing concentration of nonradiative centers. On the other hand, Ps formation was much less influenced by the band gap and nonradiative centers. Comparison of this result with that for polyethylene mixed with carbon-black nanoparticles, where a considerable reduction in Ps formation was observed, showed that nonradiative centers were of a different nature from the defects on the carbon nanoparticle surface. This work demonstrated the usefulness of positron lifetime spectroscopy combined with optical measurements to study the nanostructure of a-C:H.