Resonant two- or three-photon ionization of noble-gas atoms captured by time-resolved photoelectron momentum spectroscopy

摘要

We present an all-electron, ab initio calculation of time-resolved photoelectron momentum distributions (PMDs) induced by resonant two-color, two- or three-photon ionization of helium and neon atoms, as recently measured by Villeneuve et al. [Science 356, 1150 (2017)] using a femtosecond infrared (IR) laser pulse and an attosecond pulse train (APT) produced with high harmonic generation as an extreme ultraviolet (XUV) photon source. In contrast to a monochromatic XUV pulse commonly used at the free-electron laser facilities, an APT is broadband and ultrashort (<1 fs), so that it could induce nonresonant one-photon transitions above ionization threshold as well as a resonantly excited state. They may interfere with each other upon subsequent absorption or emission of an IR photon, so that the resultant PMD loses clear orbital symmetry. Our time-dependent density functional calculation demonstrates that the selection of a particular excited state in the time-resolved PMD is nevertheless possible if energy and timing of an APT are adjusted properly.