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Published December 21, 2014 | Published
Journal Article Open

Extension of the diffusion controlled electron transfer theory for intermittent fluorescence of quantum dots: inclusion of biexcitons and the difference of "on" and "off" time distributions

Abstract

The equations for the diffusion controlled electron transfer (DCET) theory of quantum dot blinking are extended to include biexcitons. In contrast to excitons, which under go resonant light to dark transitions, the biexcitons, having a much larger total energy, undergo a Fermi's Golden rule type transfer (many acceptance states). The latter immediately gives rise to an exponential tail for the light state, and it is explained why the dark state power law behavior is unaffected. Results are given for both continuous and pulsed excitation. The typical -3/2 power law for the light state at low light intensities, and for the dark state at all intensities, as well as dependence of the exponential tail on the square of the light intensity, and a decrease of the power in the power law for the light state from -3/2 to less negative values with increasing light intensity are all consistent with the theory. The desirability of measuring the dependence of the spectral diffusion coefficient on light intensity at room temperature as a test of several aspects of the theory is noted.

Additional Information

© 2014 the Owner Societies. Received 24 Mar 2014, Accepted 25 Apr 2014, First published online 25 Apr 2014. It is a pleasure to acknowledge the support of this research by the Office of Naval Research, the Army Research Office and the James W. Glanville Foundation, and thank Prof. Peterson for providing his experimental data.

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August 20, 2023
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