Abstract
Optical gain from colloidal quantum dots has been desired for several decades since their discovery. While gain from multiexcitations is by now well-established, nonradiative Auger recombination limits the lifetime of such population inversion in quantum dots. CdSe cores isovalently doped by one to few Te atoms capped with rod-shaped CdS are examined as a candidate system for enhanced stimulated emission properties. Emission depletion spectroscopy shows a behavior characteristic of 3-level gain systems in these quantum dots. This implies complete removal of the 2-fold degeneracy of the lowest energy electronic excitation due to the large repulsive exciton-exciton interaction in the doubly excited state. Using emission depletion measurements of the trap-associated emission from poorly passivated CdS quantum dots, we show that 3-level characteristics are typical of emission resulting from a band edge to trap state transition, but reveal subtle differences between the two systems. These results allow for unprecedented observation of long-lived population inversion from singly excited quantum dots.
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