We propose and theoretically analyze a new approach for generating and shaping 1-fs pulses. It combines the ideas of strong-field molecular optics and optimal control to manipulate light generation in a pump-probe Raman regime. Flexible phase control over the generated spectrum of about 3 eV width is achieved by controlling the input pulses and maximizing the coherence of medium excitation by adiabatically aligning molecules in the medium with a specially shaped pump pulse. The generated pulse is optimized for an output window, precompensating for its dispersion to all orders.

• Received 30 May 2001

DOI:https://doi.org/10.1103/PhysRevLett.88.103901