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We propose a methodology to design optimal pulses for achieving quantumoptimal control on molecular systems. Our approach constrains pulse shapes tolinear combinations of a fixed number of experimentally relevant pulsefunctions. Quantum optimal control is obtained by maximizing a multi-targetfitness function with genetic algorithms. As a first application of themethodology we generated an optimal pulse that successfully maximized the yieldon a selected dissociation channel of a diatomic molecule. Our pulse isobtained as a linear combination of linearly chirped pulse functions. Datarecorded along the evolution of the genetic algorithm contained importantinformation regarding the interplay between radiative and diabatic processes.We performed a principal component analysis on these data to retrieve the mostrelevant processes along the optimal path. Our proposed methodology could beuseful for performing quantum optimal control on more complex systems byemploying a wider variety of pulse shape functions.

Experimentally Attainable Optimal Pulse Shapes Obtained with the Aid of Genetic Algorithms