Restoration of coherence effects in high-power excitation of an intramolecular quasicontinuum

Israel Schek*, Joshua Jortner

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review


Three theoretical models were advanced for the dynamics of molecular multiphoton excitation: (i) The zero-order optically active mode connected by intramolecular random anharmonic couplings to a background manifold. (ii) Molecular eigenstates coupled by random radiative transition dipole moments. (iii) The kinetic master equation approach. It is demonstrated that in the Markoffian limit, as long as the intramolecular vibrational relaxation width is small relative to the Rabi frequency, these three approaches are equivalent. In the case of high-field excitation, coherent quantum effects are exhibited even in a randomly coupled system. Resurrection of the quantum oscillations and coherent pumping can be exhibited in intense field excitation on the time scale of intramolecular vibrational relaxation.

Original languageEnglish
Pages (from-to)323-335
Number of pages13
JournalTheoretica Chimica Acta
Issue number4
StatePublished - May 1986


  • Coherence effects
  • Intramolecular dynamics
  • Multiphoton excitation


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