Semiclassical guided optimal control of molecular processes of many degrees of freedom

Full-dimensional laser control of HCN-CNH isomerization is carried out to demonstrate the effectiveness of the recently formulated semiclassical guided optimal control theory. The algorithm is designed so that the controlling field does not exceed the predetermined limit of intensity to avoid the undesirable multiphoton inonization process. The controlling field is found to be rather simple and physical understanding of the controlling process becomes possible. It is demonstrated that the quantum-mechanical effects taken into account by the semiclassical treatment are essential for the control and that the purely classical treatment cannot be reliable. The theory is now applicable to any realistic molecular dynamics of many degrees of freedom.