An investigation of the effects of experimental parameters on the closed-loop control of photoionizationydissociation processes in acetophenone

The photodissociation channels of acetophenone (C H )–CO–(CH ), can be controlled by the use of tailored 6 5 3 strong-field laser pulses together with a feedback loop incorporating an adaptive algorithm. This optimal control strategy is used to selectively cleave either the OC–CH or OC–C H bonds, monitored by detecting either mass 105 3 6 5 or 77, respectively. Varying the pulse chirp and duration prior to optimization is shown to affect the dynamic range of control. We show that it is possible to decrease the search space by limiting the retardance range of the spatial light modulator (SLM), or by decreasing the number of frequency elements manipulated by the SLM, and still achieve a certain degree of control over acetophenone dissociation. Performing consecutive experiments with identical experimental parameters and search criteria reveals that the learning algorithm may find solutions that have the same degree of control (various local solutions), with either similar SLM retardances or markedly different retardances. Comparison of the dynamic range of control between single-parameter optimizations (pulse energy and duration) with the tailored electric field profiles generated by the adaptive algorithm reveals an enhancement in the control of reaction product distributions in the latter scheme. 2003 Elsevier Science B.V. All rights reserved.