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International Conference on Ultrafast Phenomena

Adiabatic Passage in the Presence of Excited-State Absorption and Two-Exciton processes

Boris D. Fainberg, Vladimir A. Gorbunov

Published Jan 1, 2006• 0 citations
Publisher

Abstract

We show that excited-state absorption has a profound effect on coherent population transfer in complex molecules that necessitates a more accurate interpretation of experimental data. A method for quantum control of two-exciton states is proposed.
DOI
10.1364/up.2006.mi12

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The influence of excited-state absorption (ESA) and two-exciton processes on a coherent population transfer with intense ultrashort chirped pulses in molecular systems in solution has been studied. A unified treatment of adiabatic rapid passage (ARP) in such systems has been developed using a three-state electronic system with relaxation treated as a diffusion on electronic potential energy surfaces. We have shown that ESA has a profound effect on coherent population transfer in large molecules that necessitates a more accurate interpretation of experimental data. A simple and physically clear model for ARP in molecules with three electronic states in solution has been developed by extending the Landau-Zener calculations putting in a third level to random crossing of levels. A method for quantum control of two-exciton states in molecular complexes has been proposed. 1.
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Abstract Transfer and manipulation of coherence among the ground state and indirect exciton states via tunneling in quadruple and multiple quantum dots is analyzed. By applying suitable amplitudes and sequences of the pump and tunneling pulses, a complete transfer of coherence or an arbitrary distribution of coherence of multiple states can be realized. The method, which is an adiabatic passage process, is different from previous works on quantum dot molecules in the way that the population can transfer from the ground state to the indirect exciton states without populating the direct exciton state, and thus no spontaneous emission occurs. This investigation can provide further insight to help the experimental development of coherence transfer in semiconductor structures, and may have potential applications in quantum information processing.