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Size-dependent intrinsic radiative decay rates of silicon nanocrystals at large confinement energies
Authors:Sykora Milan  Mangolini Lorenzo  Schaller Richard D  Kortshagen Uwe  Jurbergs David  Klimov Victor I
Affiliation:Chemistry Division, Los Alamos National Laboratory, MS-J567, Los Alamos, New Mexico 87545, USA.
Abstract:We study ultrafast photoluminescence (PL) dynamics of Si nanocrystals (NCs). The early-time PL spectra (<1 ns), which show strong dependence on NC size, are attributed to emission involving NC quantized states. The PL spectra recorded for long delays (>10 ns) are almost independent of NC size and are likely due to surface-related recombination. Based on instantaneous PL intensities measured 2 ps after excitation, we determine intrinsic radiative rate constants for NCs of different sizes. These constants sharply increase for confinement energies greater than approximately 1 eV indicating a fast, exponential growth of the oscillator strength of zero-phonon, pseudodirect transitions.
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