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Simulations of dopant pair-state distributions are presented for zincblende nanocrystals with different radii and for different dopant fractions. The probability of finding at least one pair-state and the concentration of pair-states were calculated on the basis of a statistical average of 105 simulations per crystal size and dopant concentration. The distribution of nanocrystal lattice positions over the surface and the bulk of the crystal is computed. A mathematical description of the distributions, valid in any crystal lattice, is discussed. This removes the need for further simulations.
Luminescence of nanocrystalline ZnSe:Mn2+ and ZnSe:Cu2+ prepared via an organic chemical synthesis method are described. The spectra show distinct ZnSe, Mn2+ and Cu2+ related emissions, all of which are excited via the host lattice. The Mn2+ emission wavelength depends on the concentration of Mn2+incorporated into the ZnSe lattice, which is attributed to the presence of Mn2+ pair-states at higher concentrations. The ZnSe:Cu2+ luminescence was studied as a function of the crystal-size. Temperature-dependent photoluminescence spectra and photoluminescence lifetime measurements are also presented and the results are compared to those of Mn2+ and Cu2+ in bulk ZnSe.
Nonstoichiometric precursor-ratios for the synthesis of ZnS:Mn2+ are discussed and the significant influence on the luminescence features and crystal size is explained. From the temperature quenching of the ZnS photoluminescence a luminescence excitation model is proposed. Measurements of the photoelectrochemical properties of nanocrystalline ZnS electrodes doped with Mn2+ are also presented and discussed. The observation of both anodic and cathodic photocurrent is direct evidence for the nanocrystalline nature of the system. In-situ photoluminescence measurements showed stable Mn2+ related photoluminescence over a large potential range.
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