A theory of coherent control of reaction dynamics based on the optimization of a linear time-invariant system with complex variables Original Research Article

A theory of coherent control of reaction dynamics by pulse shaping is developed based on optimization of a linear time invariant system with complex variables. This theory is an extension of a previous control theory based on a linear time-invariant system for real variables [J. Chem. Phys., 100 (1994) 5646]. The theory is successfully applied to HCN → HNC in a one dimensional model. The isomerization takes place along a minimum energy path in which several vibrational levels below the potential barrier are selected as intermediate levels. Upper two levels of them are associated with tunneling dynamics. The effects of the tunneling dynamics on the coherent isomerization are discussed.