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Pure Appl. Chem., 2000, Vol. 72, No. 1-2, pp. 245-255

Effect of atmospheric oxidation on the electronic and photoluminescence properties of silicon nanocrystal

I. N. Germanenko, M. Dongol, Y. B. Pithawalla, M. Samy El-Shall* and J. A. Carlisle

Department of Chemistry and 2 Department of Physics, Virginia Commonwealth University, Richmond, Virginia 23284 USA

Abstract: Web-like aggregates of coalesced Si nanocrystals produced by a laser vaporization-controlled condensation technique show luminescence properties that are similar to those of porous Si. The results are consistent with a quantum confinement mechanism as the source of the red photoluminescence (PL) in this system. The oxidized Si nanoparticles do not exhibit the red PL that is characteristic of the surface-oxidized Si nanocrystals. The nanoparticles are allowed to oxidize slowly, and the PL is measured as a function of the exposure time in air. A significant blue shift in the red PL peak is observed as a result of the slow oxidation process. The dependence of quantum size effects on the bonding structure is established by correlating the PL data with the photon-yield electronic structure measurements made at the Advanced Light Source. The results indicate that as the nanoparticles oxidize, the radius of the crystalline core decreases in size, which gives rise to a larger bandgap and consequently to the observed blue-shift in the PL band. The correlation between the PL, SXF, and NEXAFS results provides further support for the quantum confinement mechanism as the origin of the visible PL in Si nanocrystals.