Abstract
Carrier multiplication (CM) is a process in which absorption of a
single photon produces not just one but multiple electron-hole pairs
(excitons). This effect is a potential enabler of next-generation,
high-efficiency photovoltaic and photocatalytic systems. On the basis
of energy conservation, the minimal photon energy required to activate
CM is two energy gaps (2E(g)). Here, we analyze CM onsets for nanocrystal
quantum dots (NQDs) based upon combined requirements imposed by optical
selection rules and energy conservation and conclude that materials
with a significant difference between electron and hole effective
masses such as III-V semiconductors should exhibit a CM threshold
near the apparent 2E(g) limit. Further, we discuss the possibility
of achieving sub-2E(g) CM thresholds through strong exciton-exciton
attraction, which is feasible in NQDs. We report experimental studies
of exciton dynamics (Auger recombination, intraband relaxation, radiative
recombination, multiexciton generation, and biexciton shift) in InAs
NQDs and show that they exhibit a CM threshold near 2E(g).
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