Abstract

The concept of pump&probe spectroscopy for femtosecond chemistry [1] maybe extended to a pump&control approach for selective, vibrationally mediated, molecular transitions [2]: The first pump pulse, typically in the domain of 100 fs, induces coherent molecular vibrations either in the electronic ground [3] or excited states [1]. As a consequence, the initial configuration is changed selectively and periodically into the Franck-Condon region for the second control laser pulse which may then induce the transition to the desired product. This general strategy [1,2] is extended here to two novel applications, selective ionizations (K₂), and specific populations of barrier regions or transition states (Na₃). These simulations are carried out by wavepacket propagations on ab initio or empirical potential energy surfaces [4], see also [5].

© 1994 Optical Society of America