Probe of Multielectron Dynamics in Xenon by Caustics in High-Order Harmonic Generation

We investigated the giant resonance in xenon by high-order harmonic generation spectroscopy driven by a two-color field. The addition of a nonperturbative second harmonic component parallel to the driving field breaks the symmetry between neighboring subcycles resulting in the appearance of spectral caustics at two distinct cutoff energies. By controlling the phase delay between the two color components it is possible to tailor the harmonic emission in order to amplify and isolate the spectral feature of interest. In this Letter we demonstrate how this control scheme can be used to investigate the role of electron correlations that give birth to the giant resonance in xenon. The collective excitations of the giant dipole resonance in xenon combined with the spectral manipulation associated with the two-color driving field allow us to see features that are normally not accessible and to obtain a good agreement between the experimental results and the theoretical predictions.