Optical absorption and emission of nitrogen-doped silicon nanocrystals

Silicon nanocrystals (Si NCs) may be both unintentionally and intentionally doped with nitrogen (N) during their synthesis and processing. Since the importance of Si NCs largely originates from their remarkable optical properties, it is critical to understand the effect of N doping on the optical behavior of Si NCs. On the basis of theoretical calculations, we show that the doping of Si NCs with N most likely leads to the formation of paired interstitial N at the NC surface, which causes both the optical absorption and emission of Si NCs to redshift. But these redshifts are smaller than those induced by doubly bonded O at the NC surface. It is found that high radiative recombination rates can be reliably obtained for Si NCs with paired interstitial N at the NC surface. The current results not only help to understand the optical behavior of Si NCs synthesized and processed in N-containing environments, but also inspire intentional N doping as an additional means to control the optical properties of Si NCs.