Exciton radiative lifetime in CdSe quantum dots

Abstract

Colloidal CdSe quantum dots (QDs) are promising materials for solar cells because of their simple preparation process and compatibility with flexible substrates. The QD radiative recombination lifetime has attracted enormous attention as it affects the probability of photogenerated charges leaving the QDs and being collected at the battery electrodes. However, the scaling law for the exciton radiative lifetime in CdSe QDs is still a puzzle. This article presents a novel explanation that reconciles this controversy. Our calculations agree with the experimental measurements of all three divergent trends in a broadened energy window. Further, we proved that the exciton radiative lifetime is a consequence of the thermal average of decays for all thermally accessible exciton states. Each of the contradictory size-dependent patterns reflects this trend in a specific size range. As the optical band gap increases, the radiative lifetime decreases in larger QDs, increases in smaller QDs, and is weakly dependent on size in the intermediate energy region. This study addresses the inconsistencies in the scaling law of the exciton lifetime and gives a unified interpretation over a widened framework. Moreover, it provides valuable guidance for carrier separation in the thin film solar cell of CdSe QDs.