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Bulletin of the American Physical Society

Circular Dichroism in Atomic Resonance-Enhanced Few-Photon Ionization

Taylor J. Moon, Nicolas Douguet, Haruma Handi Nishanka De Silva, Klaus Bartschat, D. Fischer

Published Jun 3, 2021• 0 citations
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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.
The circular dichroism (CD) effect is predicted in a specific case of a two-color ionization of atoms, due to interfering a dc field-induced resonance two-photon ionization by electromagnetic radiation with frequency (omega) and the one- photon ionization by the wave with frequency 2(omega) . The maximum degree of CD may be observed in the range of fields where the probability for the dc field-induced two-photon ionization becomes comparable with that of the single-photon process and exceeds essentially the field-free two-photon ionization probability. The effect is sensitive to the relative phase between the two ac field components. The atomic parameters for this effect in alkali atoms are calculated. The range of fields is determined, for which the dichroism becomes observable. The use of the effect to control the branching ratio and the relative phase of the two radiations is discussed.