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Elsevier eBooks

Adiabatic rapid passage in molecules in solution excited by an intense ultrashort chirped pulse

Boris D. Fainberg, Vladimir A. Gorbunov

Published Jan 1, 2004• 3 citations
Publisher
DOI
10.1016/b978-044451656-5/50026-8

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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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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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Coherent population transfer in molecules coupled with a dissipative environment by intense ultrashort chirped pulse. II. A simple model

Boris D. Fainberg, Vladimir A. Gorbunov

We have developed a simple and physically clear picture of adiabatic rapid passage (ARP) in molecules in solution by careful examination of all the conditions needed for ARP. The relaxation effects were considered in the framework of the Landau-Zener model for random crossing of levels. The model enables us to include into consideration non-Markovian Gaussian-correlated noise. It explains all the numerical results obtained in the first paper of the series [B. D. Fainberg and V. A. Gorbunov, J. Chem. Phys. 117, 7222 (2002)], in particular, that for positive chirp pulse excitation relaxation favors more efficient population transfer with respect to the relaxation-free system with frozen nuclear motion. We also relate parameters of non-Markovian Gaussian-correlated noise with irreversible dephasing time of an optical transition by calculating the photon echo signal attenuation.

The Journal of Chemical Physics•Nov 2, 2004•18 citations
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.
We have developed a simple and physically clear picture of adiabatic rapid passage (ARP) in molecules in solution by careful examination of all the conditions needed for ARP. The relaxation effects were considered in the framework of the Landau-Zener model for random crossing of levels. The model enables us to include into consideration non-Markovian Gaussian-correlated noise. It explains all the numerical results obtained in the first paper of the series [B. D. Fainberg and V. A. Gorbunov, J. Chem. Phys. 117, 7222 (2002)], in particular, that for positive chirp pulse excitation relaxation favors more efficient population transfer with respect to the relaxation-free system with frozen nuclear motion. We also relate parameters of non-Markovian Gaussian-correlated noise with irreversible dephasing time of an optical transition by calculating the photon echo signal attenuation.