We report the first direct measurements of the atomic dipole phase in the process of high-order harmonic generation. Differently from previously reported studies based on frequency chirp measurements, we use extreme ultraviolet interferometry as the most natural and direct way to measure phase shifts. Our approach has the important advantage of allowing us to investigate the effects associated to both the main quantum paths involved in the emission of a particular harmonic, thus offering a particularly clear and simple picture of the underlying electronic dynamics.

Using a Ramsey-type setup, the lambda-doublet transition in the J = 1, Ω = 1 level of the a 3 Π state of CO was measured to be 394 064 870(10) Hz. In our molecular beam apparatus, a beam of metastable CO is prepared in a single quantum level by expanding CO into vacuum and exciting the molecules using a narrow-band UV laser system. After passing two microwave zones that are separated by 50 cm, the molecules are state-selectively deflected and detected 1 meter downstream on a position sensitive detector. In order to keep the molecules in a single m B J level, a magnetic bias field is applied. We find the field-free transition frequency by taking the average of the m B J = +1 → m B J = +1 and m B J = −1 → m B J = −1 transitions, which have an almost equal but opposite Zeeman shift. The accuracy of this proof-of-principle experiment is a factor of 100 more accurate than the previous best value obtained for this transition.

We demonstrate efficient generation of high-order anti-Stokes Raman sidebands in a highly transient regime, using a pair of approximately 100-fs laser pulses tuned to Raman resonance with vibrational transitions in methane or hydrogen. The use of this technique looks promising for efficient subfemtosecond pulse generation.

We have investigated the behavior of high-order stimulated Raman scattering in a highly-transient regime. We demonstrate efficient collinear generation of vibrational sidebands in molecular hydrogen and methane using two-color pumping with pulses of duration ϳ 100 fs tuned to a vibrational Raman transition. A Raman spectrum with a large bandwidth was observed, ranging from the IR to the UV. Under some conditions strong pump depletion was observed and up to five anti-Stokes sidebands were observed to have energies exceeding 10% of the transmitted pump pulse energies. A numerical simulation reproduces qualitatively and quantitatively the experimental results and allows us to explain key experimental features. The simulation also confirms that the molecular coherence in the medium is substantially increased by the two-color pumping and allows us to deduce values for the degree of material excitation. The use of this technique looks promising for efficient subfemtosecond pulse generation.