International audienceWe analyze the control of molecular orientation by nonresonant and quasiresonant two-color laser pulses (2+1 process). The laser pulses are assumed to be short with respect to the rotational period. In the nonresonant case, we show that the efficiency of this strategy crucially depends on the polarizability and the hyperpolarizability of the molecule. In the quasiresonant case, i.e., if the 2ω frequency is in quasiresonance with a vibrational frequency, one can improve the orientation by adjusting the detuning. The best orientation is obtained for an optimal value of the detuning, which is different from zero

We propose a new monotonically convergent algorithm which can enforce spectral constraints on the control field (and extends to arbitrary filters). The procedure differs from standard algorithms in that at each iteration the control field is taken as a linear combination of the control field (computed by the standard algorithm) and the filtered field. The parameter of the linear combination is chosen to respect the monotonic behavior of the algorithm and to be as close to the filtered field as possible. We test the efficiency of this method on molecular alignment. Using band-pass filters, we show how to select particular rotational transitions to reach high alignment efficiency. We also consider spectral constraints corresponding to experimental conditions using pulse shaping techniques. We determine an optimal solution that could be implemented experimentally with this technique.