Circular dichroism in atomic resonance-enhanced few-photon ionization

Abstract

We investigate few-photon ionization of lithium atoms prepared in the polarized $2p\phantom{\rule{0.16em}{0ex}}({m}_{\ensuremath{\ell}}=+1)$ state when subjected to femtosecond light pulses with left- or right-handed circular polarization at wavelengths between 665 and 920 nm. We consider whether ionization proceeds more favorably for the electric field co- or counter-rotating with the initial electronic current density. Strong asymmetries are found and quantitatively analyzed in terms of ``circular dichroism'' (CD). While the intensity dependence of the measured CD values is rather weak throughout the investigated regime, a very strong sensitivity on the center wavelength of the incoming radiation is observed. While the co-rotating situation overall prevails, the counter-rotating geometry is strongly favored around 800 nm due to the $2p\text{\ensuremath{-}}3s$ resonant transition, which can only be driven by counter-rotating fields. The observed features provide insights into the helicity dependence of light-atom interactions, and on the possible control of electron emission in atomic few-photon ionization by polarization-selective resonance enhancement.