Nearly perfect near-infrared luminescence efficiency of Si nanocrystals: A comprehensive quantum yield study employing the Purcell effect

Thin layers of silicon nanocrystals (SiNC) in oxide matrix with optimized parameters are fabricated by the plasma-enhanced chemical vapor deposition. These materials with SiNC sizes of about 4.5 nm and the SiO(2) barrier thickness of 3 nm reveal external quantum yield (QY) close to 50% which is near to the best chemically synthetized colloidal SiNC. Internal QY is determined using the Purcell effect, i.e. modifying radiative decay rate by the proximity of a high index medium in a special wedge-shape sample. For the first time we performed these experiments at variable temperatures. The complete optical characterization and knowledge of both internal and external QY allow to estimate the spectral distribution of the dark and bright NC populations within the SiNC ensemble. We show that SiNCs emitting at around 1.2–1.3 eV are mostly bright with internal QY reaching 80% at room temperature and being reduced by thermally activated non-radiative processes (below 100 K internal QY approaches 100%). The mechanisms of non-radiative decay are discussed based on their temperature dependence.