パルスレーザーを用いる化学反応の量子制御: 理論的取扱い

抄録

Quantum control utilizes coherent interactions between molecules and shaped laser pulses for driving nuclearwavepackets to the target of the reaction under investigation. Various theoretical treatments of the quantumcontrol of chemical reaction dynamics are reviewed in this paper. A general optimal control theory isintroduced to provide an understanding of the basis of quantum control of reaction dynamics. Two types ofoptimization methods, global and local are derived from the optimal control theory. An outline of a quantummechanical feedback control method developed by our group, which is a local optimization method, is brieflydescribed. The quantum mechanical feedback control theory can be used not only under weak laser field butalso under intense laser field conditions. The quantum mechanical feedback control theory is applied to simpleunimolecular reaction dynamics: ring puckering isomerization, multiphoton IR-induced dissociation of HFand predissociation of NaI. The optimized pulses are analyzed and explained in terms of π-pulses, pump anddump pulses and chirped pulses.