Optimization of field-free molecular alignment by phase-shaped laser pulses

Abstract

We theoretically demonstrate the optimization of field-free molecular alignment by phase-shaped femtosecond laser pulses. The effect is assessed in ${\mathrm{O}}_{2}$ at $T=60\phantom{\rule{0.3em}{0ex}}\mathrm{K}$ 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.