The control of molecular events by optical fields is sought with the methods of asymptotic inverse tracking, local track generation (model matching), and competitive tracking which are extensions of exact inverse tracking. The methodology is applied to infrared dissociation of a diatomic molecule and selective dissociation of the stronger bond in a highly coupled linear triatomic system. The major appeal of these methods is that they do not require costly iterations unlike other control studies in which optimization techniques are used to design fields to achieve desired molecular objectives. It is found that in exact inverse tracking where a requisite external field is obtained to exactly track a prescribed objective expectation value as a function of time, a high degree of intuition is required to find an a priori objective track such that the required fields are reasonable in terms of intensity and bandwidth. Furthermore, exact inverse tracking does not allow for tracking of multiple observables. The extensions of the inverse tracking method presented in this work help to alleviate these drawbacks. In all of these extensions the requisite field is computed locally in time through minimization of a cost functional which contains terms designed to minimize the error between the objective and actual tracks and also minimize the field fluence. The objective tracks can be prescribed a priori as in exact inverse tracking or from the present evolving system state (local track generation). Competitive tracking allows for the following of multiple observables although none will be tracked exactly. Locally generated tracks (model matching) require less physical intuition because it is easier to specify an objective track with current knowledge of the state of the system. However, the tradeoff with this method is that prediction of the behavior of the tracked observables may be elusive.
|Original language||English (US)|
|Number of pages||10|
|Journal||The Journal of chemical physics|
|State||Published - 1995|
All Science Journal Classification (ASJC) codes
- Physics and Astronomy(all)
- Physical and Theoretical Chemistry