Non-Poissonian Exciton Populations in Semiconductor Nanocrystals via Carrier Multiplication

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Abstract
We analyze distributions of exciton populations in PbSe nanocrystal (NC) ensembles as a function of excitation wavelength. For photon energies that result in carrier multiplication, these distributions are non-Poissonian and are characterized by two dominant exciton multiplicities that are determined by the ratio of photon energy to NC energy gap. For certain photon energies, we produce photoexcited NC ensembles with a nearly pure single multiplicity that can be tuned from 1 to 7. This result can find applications ranging from lasing and nonlinear optics to photovoltaics and photocatalysis.