Towards the adaptive optimization of field-free molecular alignment

We theoretically report the optimization of field-free molecular alignment by spectral phase shaping of femtosecond laser pulses. Optimal pulse shapes are designed iteratively by an evolutionary algorithm in conjunction with a non-perturbative regime calculation. The investigation is conducted in O-2 and N-2 under realistic conditions of intensity, temperature and pulse shaping. We demonstrate that specific tailored pulses can provide significant maximization of field-free alignment compared to the Fourier transform limited pulses of the same energy. The underlying control mechanism is discussed. The effect of pulse energy and temperature is analysed leading to the identification of a general criteria for a successful optimization. Finally, the optimal spectral phase learned from the algorithm is rather smooth and can be described by a representation in terms of a sigmoidal function. We show that the use of a low-dimensional parametrization of the phase yields an efficient optimization of the alignment within a highly reduced convergence time.