Electron-Hole Correlations Govern Auger Recombination in Nanostructures.

The fast nonradiative decay of multiexcitonic states via Auger recombination is a fundamental process affecting a variety of applications based on semiconductor nanostructures. From a theoretical perspective, the description of Auger recombination in confined semiconductor nanostructures is a challenging task due to the large number of valence electrons and exponentially growing number of excited excitonic and biexcitonic states that are coupled by the Coulomb interaction. These challenges have restricted the treatment of Auger recombination to simple, noninteracting electron-hole models. Herein we present a novel approach for calculating Auger recombination lifetimes in confined nanostructures having thousands to tens of thousands of electrons, explicitly including electron-hole interactions. We demonstrate that the inclusion of electron-hole correlations are imperative to capture the correct scaling of the Auger recombination lifetime with the size and shape of the nanostructure. In addition, correlation effects are required to obtain quantitatively accurate lifetimes even for systems smaller than the exciton Bohr radius. Neglecting such correlations can result in lifetimes that are two orders of magnitude too long. We establish the utility of the new approach for CdSe quantum dots of varying sizes and for CdSe nanorods of varying diameters and lengths. Our new approach is the first theoretical method to postdict the experimentally known "universal volume scaling law" for quantum dots and makes novel predictions for the scaling of the Auger recombination lifetimes in nanorods.