Publication date: 27th June 2014
After failing to detect MEG in samples of InAs core shells, and in PbSe quantum dots, using pump-probe methods, we regress to fully characterize exciton cooling dynamics in PbSe quantum dots. Spectral analysis of transient absorption using femtosecond hyperspectral near IR probing has revealed kinetically and spectrally distinct features which are incompatible with prevailing models for nanocrystal absorption and its dependence on excess energy. They appear to be at odds with the expected degeneracies of the low-lying discrete optical transitions and exhibit kinetic correlations which defy associated energy level assignments. Transient spectra of single and double hot exciton states decay with similar dynamics, arguing against the involvement of Auger cooling in the rapid exciton relaxation in PbSe QDs. In order to identify the mechanisms underlying the distinct spectral bands which accompany exciton cooling, double pump-hyperspectral probe experiments have been conducted. Preliminary results demonstrate that the sub-band gap absorption induced by excitation with high energy photons is not correlated with the 1S1S bleach, and that the assumed linearity of this bleach with the number of band edge excitons does not hold. Possible revisions of accepted models for exciton cooling in this material, which are called for by these findings, will be discussed.
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