Efficient Exciton Transport between Strongly Quantum-Confined Silicon Quantum Dots

Many-body Green function analysis and first-order perturbation theory 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 for the same center-to-center separation. This surprising result offers the prospect of designing assemblies of quantum dots through which excitons can travel for long distances, a game-changing paradigm shift for next-generation solar energy harvesting. We also find that surface reconstruction significantly influences the absorption cross section and leads to a large reduction in both transport rate and efficiency. Further, exciton transport efficiency is higher for hydrogen-passivated dots as compared with those terminated with more electronegative ligands, a result not predicted by Förster theory.