Generation of Single Intense Short Optical Pulses by Ultrafast Molecular Phase Modulation

Pulses with durations below 4 fs have been generated using the method of ultrafast molecular phase modulation. A laser pulse shorter than the molecular vibrational or rotational period obtains spectral broadening during propagation along a hollow waveguide filled with previously impulsively excited Raman active gases. The induced time dependent phase, frequency, and frequency chirp are controllable by changing the delay between excitation and probe pulse within the molecular vibrational period.