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The possibility of phase manipulation and temporal tailoring of ultrashort laser pulses provides new opportunities for optimal processing of materials. An experimental demonstration of the technique that shows the possibility to design excitation sequences tailored with respect to the material response is presented, laying the groundwork for adaptive optimization in material structuring. The technique is particularly suitable to generate controllable ion beams by ultrafast laser ablation. Silicon samples irradiated with multiple laser pulses separated by the phase-transformation time show increased ion emission efficiency with different energetic signatures correlated to a cleaner aspect of the laser-induced structures on the surface. © 2003 American Institute of Physics.