New way of controlling molecular processes by time-dependent external fields

A new idea of controlling molecular processes by time-dependent external fields is proposed. Molecular processes in external fields are considered to be composed of a sequence of time-dependent nonadiabatic transitions in which the external fields play a role of adiabatic parameters. Unit final transition probability can be achieved with the use of the interference effects among various paths created by nonadiabatic transitions. The basic idea is to sweep the external field periodically at each avoided crossing and to control the transition there completely as we desire. This idea is quite general, and can hold whatever the external field is. Various control schemes can be proposed corresponding to the various types of time-dependent nonadiabatic transitions. The methods of π-pulse and chirped laser pulse with the adiabatic rapid passage may be considered as special cases of the present idea. As an example, a one-dimensional model of the laser-induced ring-puckering isomerization of trimethylenimine is considered, and comparative studies on the effectiveness and the stability of the various control schemes proposed in this paper are made together with presentation of numerical examples.