Aerosol-Phase Synthesis and Processing of Luminescent Silicon Nanocrystals

Silicon quantum dots are attractive materials for luminescent devices and bioimaging applications. For these light-emitting applications, higher photoluminescence efficiency is desired in order to achieve better device performance. Nonthermal plasma synthesis successfully allows for the continuous production of silicon nanocrystals, but postprocessing is necessary to improve photoluminescence quantum yields so that nanocrystals can be used for luminescence applications. In this work, we demonstrate an all-aerosol-phase synthesis and processing route that integrates nonthermal plasma synthesis, plasma-assisted surface functionalization with alkene ligands, and in-flight annealing within one flow stream. Here, luminescent silicon nanocrystals are synthesized and postprocessed on a time scale of only 100 ms, which is orders of magnitude faster than previous synthesis and functionalization schemes. The as-produced silicon nanocrystals have photoluminescence quantum yields exceeding 20%, which is a 5-fold increase compared to previous silicon nanocrystals synthesized with all-aerosol-phase approaches. We attribute the enhanced photoluminescence to the reduced "dark" nanocrystal fraction due to reduction of dangling bond density and desorption of surface silyl species induced by the in-flight annealing. We also demonstrate that the ligand coverage plays a minor role for the photoluminescence properties, but that the nature of the silicon hydride surface groups is a major factor.