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An atomistic pseudopotential method is used to investigate the electronic and optical properties of spherical InAs nanocrystals. Our calculated interband (valence-to-conduction) absorption spectra reproduce the features observed experimentally both qualitatively and quantitatively. The results relative to intraband (valence-to-valence and conduction-to-conduction) absorption successfully reproduce the recently measured photoinduced absorption spectra, which had so far been addressed only qualitatively. They exclude the hypothesis of a thermal activation process between dot-interior-delocalized hole states to explain the temperature dependence observed experimentally. Furthermore, based on the agreement of our data with the experimental valence intersublevel transitions and the almost complete overlap of the latter with scanning tunneling microscopic (STM) measurements, we question the simplistic attribution of the observed STM peaks obtained for negative bias.

Interband and intraband optical transitions in InAs nanocrystal quantum dots: A pseudopotential approach