Carrier dynamics in Si nanocrystals in an SiO<inf>2</inf> matrix investigated by transient light absorption

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Journal Article
Physical Review B - Condensed Matter and Materials Physics, 2013, 88 (15)
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We report on investigations of optical carrier generation in silicon nanocrystals embedded in an SiO2 matrix. Carrier relaxation and recombination processes are monitored by means of time-resolved induced absorption, using a conventional femtosecond pump-probe setup for samples containing different average sizes of nanocrystals (dNC = 2.5-5.5 nm). The electron-hole pairs generated by the pump pulse are probed by a second pulse over a broad spectral range (Eprobe = 0.95-1.35 or 1.6-3.25 eV), by which information on excited states is obtained. Under the same excitation conditions, we observe that the induced absorption intensity in the near-infrared range is a factor of ∼10 higher than in the visible range. To account for these observations, we model the spectral dependence of the induced absorption signal using an empirical sp3d5s* tight-binding technique, by which the spectrum can be well reproduced up to a certain threshold. For probe photon energies above this threshold (dependent on nanocrystal size), the induced absorption signal is found to feature a long-standing component, whereas the induced absorption signal for probe photon energies below this value vanishes within 0.5 ns. We explain this by self-trapping of excitons on surface-related states. © 2013 American Physical Society.
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