RESUMEN
As the commercial display market grows, the demand for low-toxicity, highly emissive, and size-tunable semiconducting nanoparticles has increased. Indium phosphide quantum dots represent a promising solution to these challenges; unfortunately, they typically suffer from low inherent emissivity resulting from charge carrier trapping. Strategies to improve the emissive characteristics of indium phosphide often involve zinc incorporation into or onto the core itself and the fabrication of core/shell heterostructures. InP clusters are high fidelity platforms for studying processes such as cation exchange and surface doping with exogenous ions since these clusters are used as single-source precursors for quantum dot synthesis. Here, we examined the incorporation of zinc and gallium ions in InP clusters and the use of the resultant doped clusters as single-source precursors to emissive heterostructured nanoparticles. Zinc ions were observed to readily react with InP clusters, resulting in partial cation exchange, whereas gallium resisted cluster incorporation. Zinc-doped clusters effectively converted to emissive nanoparticles, with quantum yields strongly correlated with zinc content. On the other hand, gallium-doped clusters failed to demonstrate improvements in quantum dot emission. These results indicate stark differences in the mechanisms associated with aliovalent and isovalent doping and provide insight into the use of doped clusters to make emissive quantum dots.
RESUMEN
Doping of semiconductors by impurity atoms enabled their widespread technological application in microelectronics and optoelectronics. However, doping has proven elusive for strongly confined colloidal semiconductor nanocrystals because of the synthetic challenge of how to introduce single impurities, as well as a lack of fundamental understanding of this heavily doped limit under strong quantum confinement. We developed a method to dope semiconductor nanocrystals with metal impurities, enabling control of the band gap and Fermi energy. A combination of optical measurements, scanning tunneling spectroscopy, and theory revealed the emergence of a confined impurity band and band-tailing. Our method yields n- and p-doped semiconductor nanocrystals, which have potential applications in solar cells, thin-film transistors, and optoelectronic devices.
RESUMEN
Tunable femtosecond pump-near IR probe measurements on InAs/CdSe/ZnSe core/shell1/shell2 nanocrystal quantum dots were conducted to quantify spontaneous carrier multiplication previously reported in this system. Experimental conditions were chosen to eliminate the need for determining absolute wavelength dependent cross sections of the nanocrystals and allow direct comparison of band edge absorption bleach kinetics for different excitation energies up to 3.7 times the band gap. Results for two sample sizes show no signs of carrier multiplication within that range. This result is discussed in light of reports describing occurrence of this novel phenomenon in quantum dots based on this as well as numerous other semiconductor materials.