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Superlattices of Si-rich silicon nitride and Si 3 N 4 are prepared by plasma-enhanced chemical vapor deposition and, subsequently, annealed at 1150 C to form size-controlled Si nanocrystals (Si NCs) embedded in amorphous Si 3 N 4. Despite well defined structural properties, photoluminescence spectroscopy (PL) reveals inconsistencies with the typically applied model of quantum confined excitons in nitride-embedded Si NCs. Time-resolved PL measurements demonstrate 10 5 times faster time-constants than typical for the indirect band structure of Si NCs. Furthermore, a pure Si 3 N 4 reference sample exhibits a similar PL peak as the Si NC samples. The origin of this luminescence is discussed in detail on the basis of radiative defects and Si 3 N 4 band tail states in combination with optical absorption measurements. The apparent absence of PL from the Si NCs is explained conclusively using electron spin …