Diffusion properties of chalcogens (S, Se, Te) into pure silica

Université Paris-Sud 11, Orsay, Île-de-France, France
Journal of Non-Crystalline Solids (Impact Factor: 1.77). 10/2005; 351(37-39):3031-3036. DOI: 10.1016/j.jnoncrysol.2005.07.011


The diffusion properties of chalcogens (S, Se, Te) implanted into SiO2 were studied via secondary ion mass spectroscopy (SIMS) profiling between room temperature and the glass transition temperature (800–950 °C). Annealing of Te-containing samples leads directly to precipitation of metallic tellurium nanocrystals within the implantation profile. The S and Se concentration profiles were fitted by using a simple diffusion model in order to provide estimates of the diffusion constant and approximate solubility of these fast moving chemical species. A comparison of their differing diffusion behavior with complementary data on these systems suggests that (i) their oxidation states play a crucial role and (ii) the chalcogen propagation mechanism actually involves complex chemical interactions.

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    ABSTRACT: Lead chalcogenide (PbS, PbSe, and PbTe) nanocrystals were synthesized by sequential implantation of Pb and one of the chalcogen species into pure silica. The implantation energy and fluence were chosen so that the implantation profiles practically overlap at a depth approximately 150 nm with a maximum concentration of about 0.3 atom %. Annealing for 1-8 h at 850-900 degrees C triggers nanocrystal growth, which is monitored by high-resolution (HRTEM) and conventional transmission electron microscopy (TEM), secondary-ion mass spectrometry (SIMS), and Rutherford backscattering spectrometry (RBS). Striking differences are found in the depth distributions and microstructures of the resulting nanocrystals. We show that the differing chemical interactions of Pb and chalcogens (between each other and with silica) play a crucial role in chalcogenide nucleation and growth. Using available information on chalcogen redox states in silicate glass, we propose a nonclassical nucleation and growth mechanism consistent with our experimental results. The complex chemistry involved at the microscopic level is shown to impair control over the nanocrystal size distribution. Finally, PbS nanocrystal-doped silica is shown to emit intense photoluminescence (PL) in the 1.5-2 microm wavelength range, an effect that we relate to the above nucleation and growth scheme.
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