Femtosecond pump-probe fluorescence signals from classical trajectories: comparison with wave-packet calculations |
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| Authors: | VA Ermoshin V Engel |
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| Institution: | Fock Institute of Physics, The University of St. Petersburg, 198504 St. Petersburg, Russia, RU
Institut für Physikalische Chemie, Universit?t Würzburg, Am Hubland, 97074 Würzburg, Germany, DE
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| Abstract: | A classical approach to simulate femtosecond pump-probe experiments is presented and compared to the quantum mechanical treatment.
We restrict the study to gas-phase systems using the I2 molecule as a numerical example. Thus, no relaxation processes are included. This allows for a direct comparison between
purely quantum mechanical results and those obtained from classical trajectory calculations. The classical theory is derived
from the phase-space representation of quantum mechanics. Various approximate quantum mechanical treatments are compared to
their classical counterparts. Thereby it is demonstrated that the representation of the radial density as prepared in the
pump-process is most crucial to obtain reliable signals within the classical approach.
Received 28 March 2001 |
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| Keywords: | PACS 31 70 Hq Time-dependent phenomena: excitation and relaxation processes and reaction rates – 33 80 Wz Other multiphoton processes |
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