We report that high-order harmonic generation (HHG) of atoms driven by ω-2ω bi-elliptical pumps exhibits a substantial sensitivity to variation of the spatial extent of the participating valence orbitals and effective potential. We identify the physical mechanisms responsible for this enhanced sensitivity through theoretical investigations in atomic He, Ne, Ar, and Kr systems using several quantum models. We demonstrate this size sensitivity experimentally by measuring significant disparities in the bi-elliptical HHG spectra of atomic Ar and Kr, which have relatively similar ionization potentials, but substantially different p-shell sizes and effective potentials. This result may be useful for ultrafast spectroscopy which is sensitive to effective potentials and orbitals.
|Journal||Physical Review A|
|State||Published - 25 Oct 2019|