Colloidal semiconductor quantum dots are fluorescent nanocrystals exhibiting exceptional optical properties, but their emission intensity strongly depends on their charging state and local environment. This leads to blinking at the single-particle level or even complete fluorescence quenching, and limits the applications of quantum dots as fluorescent particles. Here, we show that a single quantum dot encapsulated in a silica shell coated with a continuous gold nanoshell provides a system with a stable and Poissonian emission at room temperature that is preserved regardless of drastic changes in the local environment. This novel hybrid quantum dot/silica/gold structure behaves as a plasmonic resonator with a strong Purcell factor, in very good agreement with simulations. The gold nanoshell also acts as a shield that protects the quantum dot fluorescence and enhances its resistance to high-power photoexcitation or high-energy electron beams. This plasmonic fluorescent resonator opens the way to a new family of plasmonic nanoemitters with robust optical properties.
We study the synthesis of indium phosphide quantum dots using InCl 3 , tris(dimethylamino)phosphine (P-(NMe 2 ) 3 ), and oleylamine. We optimized the reaction conditions to reach high chemical yield (∼70%) and size control of the quantum dots with absorption maxima over all the visible range. Kinetic studies of the formation of the quantum dots show that, under certain conditions, the growth of nanoparticles seems to approach a LaMer type growth. We have used 31 P NMR, mass spectroscopy, and DFT calculations to decipher the reaction mechanisms of InP formation at the molecular level. The mechanistic investigation is in good agreement with the conclusions drawn from the optimization of the synthetic conditions.
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