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Conical intersections (CIs) have been widely studied using spectroscopictechniques. However, CIs have mainly been identified by rapid internalconversion transitions that take place after the photoexcitation. Suchidentifications cannot distinguish various types of intersections as well as toseparate the actual intersection from an avoided crossing. In this paper, weinvestigate how ultrafast IR laser pulses can be utilized to stimulate nucleardynamics revealing geometric phase features associated with CIs. We considertwo low-dimensional nonadiabatic models to obtain optimal two- and three-pulselaser sequences for stimulating nuclear dynamics necessary for the CIidentification. Our results provide insights on designing non-linearspectroscopic schemes for subsequent probes of the nuclear wavepackets byultrafast electron diffraction techniques to unambiguously detect CIs inmolecules.

chemical physics

Exploring vibrational ladder climbing in vibronic coupling models:  Toward experimental observation of a geometric phase signature of a conical  intersection