Optimal generation of single-dispersion precompensated 1-fs pulses by molecular phase modulation.

We show how an optimal control approach can be combined with the pump-probe technique for pulse compression by molecular phase modulation in hollow-core fibers to generate single 1-fs pulses in the visible. Varying the intensity and duration of the Gaussian-shaped pump pulse at the input induces optimal rotational response of the molecules. The probe pulse, which scatters off of the resulting time variation of the refractive index, is shaped at the input for optimal compression at the output, including dispersion to all orders.