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Hydrogen passivation of Si nanocrystals is shown to result in a redshift of photoluminescence (PL) emission spectra, as well as the more commonly observed intensity increase. The shift is reversible, with spectra returning to their unpassivated values as hydrogen is removed from the samples by annealing. The magnitude of the redshift also depends on the implant fluence employed for nanocrystal synthesis, increasing with increasing fluence or particle size. These data are shown to be consistent with a model in which larger crystallites are assumed to contain a greater number of nonradiative defects, i.e., the number of nonradiative defects is assumed to scale with the surface area or volume of a nanocrystal. Hydrogen passivation then results in a disproportionate increase in emission from larger crystallites, giving rise to an apparent redshift in the composite PL emission spectrum. © 2001 American Institute of Physics.