Adiabatic passage in a three-state system with non-Markovian relaxation: the role of excited-state absorption and two-exciton processes |
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Authors: | Fainberg B D Gorbunov V A |
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Affiliation: | Faculty of Sciences, Physics Department, Holon Institute of Technology, 52 Golomb Street, Holon 58102, Israel. fainberg@hit.ac.il |
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Abstract: | 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. |
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