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We present a self-contained theoretical and computational framework fordynamics following photoexcitation in quantum dots near planar interfaces. Amicroscopic Hamiltonian parameterized by first principles calculations ismerged with a reduced density matrix formalism that allows for the predictionof time-dependent charge and energy transfer processes between the quantum dotand the electrode. While treating charge and energy transfer processes on anequal footing, the non-perturbative effects of sudden charge transitions on theFermi sea of the electrode are included. We illustrate the formalism withcalculations of an InAs quantum dot coupled to the Shockley state on an Au[111]surface, and use it to concretely discuss the wide range of kinetics possiblein these systems and their implications for photovoltaic systems and tunneljunction devices. We discuss the utility of this framework for the analysis ofrecent experiments.

Microscopic theory to quantify the competing kinetic processes in photoexcited surface-coupled quantum dots