We theoretically demonstrate the optimization of field-free molecular alignment by phase-shaped femtosecond laser pulses. The effect is assessed in O-2 at T=60 K under realistic conditions of intensity and pulse shaping. The spectral laser phase is sampled through 128 control parameters and a self-learning evolutionary algorithm combined with a nonperturbative regime calculation is used in order to design the specific phase that maximizes the degree of alignment. The postpulse molecular alignment appears significantly enhanced compared to a Fourier-transform-limited pulse of same energy. The analysis of the target state reveals that the solution is close to the optimal one.
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