Ternary CdS x Te 1-x semiconductor quantum dots with both homogeneous and gradient composition have been fabricated via pyrolysis of organometallic precursors. The nanocrystal structure, size, and composition were characterized by UV-visible absorption and fluorescence spectroscopy, transmission electron microscopy, energy-dispersive X-ray elemental analysis, and X-ray diffractrometry. It was found that the band gap of homogeneously alloyed CdS x Te 1-x is highly nonlinear with the crystalline composition, which was evidenced by a significant red-shift in the fluorescence of these nanocrystals with respect to the emission wavelength of their CdS and CdTe binary compounds. This effect, also known as optical bowing, seems to be enhanced in CdS x Te 1-x nanocrystals because of large differences in atomic radii and electronegativities of S and Te chalcogens. Properties of gradient ternary alloys were found to be markedly different from those of homogeneous CdS x Te 1-x. Their absorption and emission profiles, for instance, had a relatively low spectral overlap leading to large Stokes shifts of up to 150 nm. Other properties of fabricated CdS x Te 1-x nanocrystals and their significance to applications in areas of biomedical imaging, solar cells, and quantum dot-based LEDs are discussed.
Properties of colloidal heterostructured nanocrystals are largely determined by the spatial distribution of photogenerated carriers across the junction of semiconductor materials that form the heterostructure. The two known types of carrier distributions are identified based on whether both carriers reside within the same (type I) or opposite (type II) sides of the heterojunction. Here we demonstrate the existence of another type of spatial carrier distribution in heteronanocrystals, which corresponds to the localization of both charges along the material junction. Such localization pattern was realized in novel CdTe/ZnSe heteronanocrystals, where the expected type I infrared emission was dominated by more intense photoluminescence in the 570-600 nm range, corresponding to the recombination of carriers within an interfacial alloy layer, formed by the cation and anion exchange between CdTe and ZnSe phases. Fabricated heteronanocrystals exhibit excellent optical characteristics including near-single-exponential lifetimes, enhanced emission stability, and fluorescence emission quantum yields of up to 24%.
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