To understand and optimize optical spin initialization in room temperature CdSe nanocrystal quantum dots (NCQDs) we studied the dependence of the time-resolved Faraday rotation signal on pump energy $E_p$ in a series of NCQD samples with different sizes. In larger NCQDs, we observe two peaks in the spin signal vs. $E_p$, whereas in smaller NQCDs, only a single peak is observed before the signal falls to a low, broad plateau at higher energies. We calculate the spin-dependent oscillator strengths of optical transitions using a simple effective mass model to understand these results. The observed $E_p$ dependence of the spin pumping efficiency (SPE) arises from the competition between the heavy hole (hh), light hole (lh) and split-off (so) band contributions to transitions to the conduction band. The two latter contributions lead to an electron spin polarization in the opposite direction from the former. At lower $E_p$ the transitions are dominated by the hh band, giving rise to the low energy peaks. At higher $E_p$, the increasing contributions from the lh and so bands lead to a reduction in SPE. The different number of peaks in larger and smaller NCQDs is attributed to size-dependence of the ordering of the valence band states.
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