Efficient Exciton Transport in Strongly Quantum-Confined Silicon Quantum Dots

Abstract

First-order perturbation theory and many-body Green function analysis are used to quantify the influence of size, surface reconstruction and surface treatment on exciton transport between small silicon quantum dots. Competing radiative processes are also considered in order to determine how exciton transport efficiency is influenced. The analysis shows that quantum confinement causes small (~1 nm) Si quantum dots to exhibit exciton transport efficiencies far exceeding that of their larger counterparts. We also find that surface reconstruction significantly influences the absorption cross section and leads to a large reduction in both transport rate and efficiency. Exciton transport efficiency is higher for hydrogen passivated dots as compared with those terminated with more electronegative ligands. This is because such ligands delocalize electron wave functions towards the surface and result in a lower dipole moment. Such behavior is not predicted by F\"orster theory, built on a dipole-dipole approximation, because higher order multi-poles play a significant role in the exciton dynamics.