Abstract
We study the coherent mixing between two-particle (single exciton) and four-particle (biexciton) states of a semiconductor nanocrystal resulting from the Coulomb coupling between states with different numbers of electron-hole pairs. Using a simple model of the nanocrystal wave functions and an envelope function approach, we estimate the efficiency of the multiple exciton generation (MEG) process resulting from such coherent admixture mechanism, including all the relevant states in a very broad energy interval. We show that in a typical ensemble of nanocrystals with an average radius of 3nm, the onset of the MEG process appears about 1 eV above the lower edge of the biexciton density of states. This is due to the angular momentum conservation that imposes selection rules and limits the available MEG pathways, thus taking over the role of momentum conservation that hinders this process in bulk. The efficiency of the MEG process reaches 50% for photon energies around 5 eV. The MEG onset shifts to lower energies and therefore the efficiency increases in a certain energy range as the radius grows. The energy dependence of the MEG efficiency differs considerably between ensembles with small and large inhomogeneity of nanocrystal sizes.
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