Excitonic effects and optical properties of passivated CdSe clusters

Details Excitonic effects and optical properties of passivated CdSe clusters Excitonic effects and optical properties of passivated CdSe clusters

2006-08-24

arxiv.org/abs/cond-mat/0608521v1

Physics

Condensed Matter

Materials Science

4 pages, to appear in Phys. Rev. Lett

Scientific paper

We calculate the optical properties of a series of passivated non-stoichiometric CdSe clusters using two first-principles approaches: time-dependent density functional theory within the local density approximation, and by solving the Bethe-Salpeter equation for optical excitations with the GW approximation for the self-energy. We analyze the character of optical excitations leading to the first low-energy peak in the absorption cross-section of these clusters. Within time-dependent density functional theory, we find that the lowest-energy excitation is mostly a single-level to single-level transition. In contrast, many-body methods predict a strong mixture of several different transitions, which is a signature of exciton effects. We also find that the majority of the clusters have a series of dark transitions before the first bright transition. This may explain the long radiative lifetimes observed experimentally

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