Type-II core/shell CdS/ZnSe nanocrystals: synthesis, electronic structures, and spectroscopic properties - PubMed (original) (raw)
. 2007 Sep 26;129(38):11708-19.
doi: 10.1021/ja068351m. Epub 2007 Aug 30.
Affiliations
- PMID: 17727285
- DOI: 10.1021/ja068351m
Type-II core/shell CdS/ZnSe nanocrystals: synthesis, electronic structures, and spectroscopic properties
Sergei A Ivanov et al. J Am Chem Soc. 2007.
Abstract
We report a two-step synthesis of highly luminescent CdS/ZnSe core/shell nanocrystals (emission quantum yields up to 50%) that can produce efficient spatial separation of electrons and holes between the core and the shell (type-II localization regime). Our synthesis involves fabrication of cubic-singony CdS core particles that are subsequently overcoated with a layer of ZnSe in the presence of surfactant-ligands in a noncoordinating solvent. Studies of different growth regime of the ZnSe shell indicate that one approach to obtaining high emission efficiencies is through alloying the CdS/ZnSe interface with CdSe, which leads to the formation of an intermediate ZnCdSe layer with a graded composition. We perform theoretical modeling of these core/shell nanocrystals using effective mass approximation and applying first-order perturbation theory for treating both direct electron-hole coupling and the core/shell interface-polarization effects. Using this model we determine the range of geometrical parameters of the core/shell structures that result in a type-II localization regime. We further applied this model to evaluate the degree of electron-hole spatial separation (quantified in terms of the electron-hole overlap integral) based on measured emission wavelengths. We also discuss the potential applicability of these nanocrystals in lasing technologies and specifically the possibility of single-exciton optical gain in type-II nanostructures.
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