Abstract

A theoretical description of stimulated-emission pumping with femtosecond laser pulses on complex absorption bands of polyatomic molecules is developed. The strong non-Born–Oppenheimer coupling associated with conical intersections of multidimensional excited-state potential-energy surfaces is included in a fully microscopic manner for appropriate model systems. Additional relaxation effects in the excited-state manifold (lifetime broadening and pure dephasing) are included in the usual phenomenological manner by using the density-matrix formalism. The calculation of the stimulated-emission pump–probe signal by means of density-matrix perturbation theory is briefly discussed and numerically realized using a time-dependent eigenstate-free treatment of the intramolecular dynamics. Some results obtained for a simple model of the S1S2 conical intersection in pyrazine are presented.

© 1990 Optical Society of America

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