Time-correlated single-photon counting study of multiple photoluminescence lifetime components of silicon nanoclusters

We report time-resolved photoluminescence measurements of thin films of silica containing silicon nanoclusters (Si NCs), produced by PECVD and annealed at temperatures between 700 °C and 1150 °C. While the near infrared emission of Si NCs has long been studied, visible light emission has only recently attracted interest due to its very short decay times and its recently-reported redshift with decreasing NCs size. We analyse the PL decay dynamics in the range 450-700 nm with picosecond time resolution using Time Correlated Single Photon Counting. In the resultant multi-exponential decays two dominant components can clearly be distinguished: a very short component, in the range of hundreds of picoseconds, and a nanosecond component. In this wavelength range we do not detect the microsecond component generally associated with excitonic recombination. We associate the nanosecond component to defect relaxation: it decreases in intensity in the sample annealed at higher temperature, suggesting that the contribution from defects decreases with increasing temperature. The origin of the very fast PL component (ps time region) is also discussed. We show that it is consistent with the Auger recombination times of multiple excitons. Further work needs to be done in order to assess the contribution of the Auger-controlled recombinations to the defect-assisted mechanism of photoluminescence. © 2012 Elsevier B.V. All rights reserved.