The location and size distribution of silicon nanocrystals ͑Si-nc͒ formed in SiO 2 by Si ion implantation and annealing were investigated. Transmission electron microscopy images revealed that the location and size distribution of the Si-nc are strongly correlated with the location of the vacancies produced in the SiO 2 network by the implantation, as simulated by stopping and range of ions in matter and measured by positron annihilation spectroscopy ͑PAS͒. Simultaneous consideration of PAS and photoluminescence measurements suggest that the diffusion necessary for Ostwald ripening of Si-nc depends on the concentration and location of vacancy-type defects, and when the majority of these defects have been removed by annealing, the growth of the Si-nc slows dramatically or stops entirely. We demonstrate the capability for modification and enhancement of emission from Si-nc through the controlled introduction of defects into the oxide prior to annealing.

Luminescence of amorphous Si quantum dots (Si QDs) in a hydrogenated silicon nitride (SiNx:H) matrix was examined over a broad range of stoichiometries from Si3N2.08 to Si3N4.14, to optimize light emission. Plasma-enhanced chemical vapor deposition was used to deposit hydrogenated SiNx films with excess Si on Si (001) substrates, with stoichiometry controlled by variation of the gas flow rates of SiH4 and NH3 gases. The compositional and optical properties were analyzed by Rutherford backscattering spectroscopy, elastic recoil detection, spectroscopic ellipsometry, photoluminescence (PL), time-resolved PL, and energy-filtered transmission electron microscopy. Ultraviolet-laser-excited PL spectra show multiple emission bands from 400 nm (3.1 eV) to 850 nm (1.45 eV) for different Si3Nx compositions. There is a red-shift of the measured peaks from ∼2.3 eV to ∼1.45 eV as Si content increases, which provides evidence for quantum confinement. Higher N content samples show additional peaks in their PL spectra at higher energies, which we attribute to defects. We observed three different ranges of composition where Tauc band gaps, PL, and PL lifetimes change systematically. There is an interesting interplay of defect luminescence and, possibly, small Si QD luminescence observed in the intermediate range of compositions (∼Si3N3.15) in which the maximum of light emission is observed.

Time-resolved photoluminescence measurements of silicon nanocrystals formed by ion implantation of silicon into silicon dioxide reveal multi-exponential luminescence decays. Three discrete time components are apparent in the rise and decay data, which we associate with different classes of nanocrystals. The values of decay time are remarkably constant with emission energy, but the relative contributions of the three components vary strongly across the luminescence band. In keeping with the quantum confinement model for luminescence, we assign emission at high energies to small nanocrystals and that at low energies to large nanocrystals. By deconvolving the decay data over the full emission band, it is possible to study the migration of excitation from smaller (luminescence donor) to larger (luminescence acceptor) nanocrystals. We propose a model of diffusion of excitation between neighboring nanocrystals, with long lifetime emission being from the largest nanocrystal in the local neighborhood. Our data also allow us to study the saturation of acceptor nanocrystals, effectively switching off excitation transfer, and Auger recombination in non-interacting nanocrystals.

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