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
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