Impact Ionization Can Explain Carrier Multiplication in PbSe Quantum Dots

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Abstract
The efficiency of conventional solar cells is limited because the excess energy of absorbed photons converts to heat instead of producing electron−hole pairs. Recently, efficient carrier multiplication has been observed in semiconductor quantum dots. In this process, a single, high-energy photon generates multiple electron−hole pairs. Rather exotic mechanisms have been proposed to explain the efficiency of carrier multiplication in PbSe quantum dots. Using atomistic pseudopotential calculations, we show here that the more conventional impact ionization mechanism, whereby a photogenerated electron−hole pair decays into a biexciton in a process driven by Coulomb interactions between the carriers, can explain both the rate (≪1 ps) and the energy threshold (∼2.2 times the band gap) of carrier multiplication, without the need to invoke alternative mechanisms.