Aqueous Synthesis of Thiol-Capped CdTe Nanocrystals:  State-of-the-Art

Abstract

We report on the state-of-the art synthesis and improved luminescence properties of thiol-capped CdTe nanocrystals (NCs) synthesized in water. The optimized pH (12) and molar ratio of thiol to Cd ions (1.3:1) increases the room-temperature photoluminescence quantum efficiency of as-synthesized CdTe NCs capped by thioglycolic acid (TGA) to values of 40−60%. By employing mercaptopropionic acid (MPA) as a stabilizer, we have synthesized large (up to 6.0 nm in diameter) NCs so that the spectral range of the NCs' emission currently available within this synthetic route extends from 500 to 800 nm. Sizing curve for thiol-capped CdTe NCs is provided. In contrast to CdTe NCs capped by TGA, MPA-capped CdTe NCs show up to 1 order of magnitude longer (up to 145 ns) emission decay times, which become monoexponential for larger particles. This phenomenon is explained by considering the energetics of the Te-related traps in respect to the valence-band position of CdTe NCs. The correlation between luminescence quantum efficiencies, luminescence lifetimes, and Stokes shifts of CdTe NC fractions is demonstrated, being in agreement with a model proposed previously that connects the emission properties of NCs with their surface quality determined by the Oswald ripening conditions during growth. imaging, and plasmonics.