A novel single-precursor nanoparticle growth technique for luminescent metal sulfides (cadmium sulfide, lead sulfide, zinc sulfide) with hydrophilic surface modification.

摘要

In recent years luminescent semiconductor nanoparticles (quantum dots) have attracted considerable attention, mostly due to their size-dependent tunable spectroscopic properties. Currently, fluorescing particles are put to use as biological labels alongside, or even replacing, fluorescing molecular probes. They are characterized by very narrow and tunable (excitonic) emission bands and long-range stability even under illumination. In particular, the colloidal chemistry approach to luminescent nanoparticle fabrication has been favored due to its relative ease, and high size tunability. However, the development of highly monodisperse, size tunable, and highly stable aqueous colloidal suspension fabrication methodologies has to date been very limited. In this work, the synthesis of luminescent MS (M = Cd, Pb, Zn) nanoparticles was achieved through the development and implementation of three characteristically different reaction methodologies: a spontaneous precipitation reaction (the metal chloride method), a controlled precipitation reaction (the metal oxide method), and a novel controlled aqueous decomposition reaction (the metal ethyl xanthate method) in an alkylamine solvent of 4-dimethylaminopyridine (DMAP). Varying degrees of monodispersity were achieved for the various methods, as evidenced by the photoluminescence full-width at half-maximum (FWHM). Spectral widths range from 150 nm for spontaneous precipitation methods, to as small as 20 nm for each of the temperature-controlled nucleation and ripening methods. For each of the methods, attempts at size tunability through variation of precursor concentration, growth temperature and growth time were performed. This resulted in the demonstration of an ability to fabricate size-specified semiconducting nanoparticles in the sub-10 nm size range. A demonstration of aqueous-organic-aqueous phase transfer versatility of the metal ethyl xanthate-DMAP fabrication method advances the potential of this particular method for many applications, including biological, microelectronic, and optoelectronic use.