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77953308594
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note
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In the case of Poisson statistics, for an average degree of photocharging of 0.25 the fraction of doubly charged NCs is only ∼2%. The actual fraction of such NCs should be even lower as the existence of one charge in a NC complicates the introduction of the second charge because of an additional Coulombic barrier. This effect is expected to lower the probability of double charging compared to that for Poisson statistics.
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The assumption that the efficiency of CM is the same in charged and neutral NCs is at odds with the results of a recent computation (ref 39) but is supported by the fact that this assumption produces good quantitative agreement between the CM results for stirred samples and the true CM efficiencies extracted from the apparent CM yields in static measurements. Another piece of evidence that photocharging does not suppress CM is the appearance in static samples of a PL relaxation component faster than that of a neutral biexciton when the corresponding stirred sample only shows decay characteristic of neutral biexcitons.
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40
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The derivation of the degree of photocharging from time-integrated PL measurements is based on the assumption that the Auger lifetime of charged species (excitons and biexcitons) is much shorter than their radiative decay times, and hence, the time-integrated signal is dominated by emission from neutral NCs. Indeed, we always observe a reduction in time-integrated emission intensity upon stopping the stirring of samples that show a static-stirred difference in PL dynamics. Further, we see good quantitative agreement between fractional changes in the time-integrated PL and long-time PL signals measured by PL up-conversion.
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