<p>  Based on the multichannel quantum defect method and streamlined R-matrix treatment, this thesis studies the multi-photon ionization spectrum for atomic helium and barium, and explores the electronic correlations of these atoms. For the helium atom, the above-threshold-ionization spectra have been calculated, with two linearly polarized photons, two oppositely circularly polarized photons, and three linearly polarized photons. The propensity rules for the single-photon ionization and autoionizing decay have been extended into the multi-photon region, showing that the excitation rules are not always satisfied for the most prominent channel. In a separate project, based on the spontaneous two-photon decay of the helium 1s2s 1Se excited state that has a rather long lifetime, one can create photon pairs that are entangled in time, frequency, and polarization. Experimental schemes are proposed to use them as a laser source to ionize another helium. Finally, we considered the oneand two-photon pathway coherent control of atomic helium and barium near their autoionizing levels. For the helium atom, we proposed a controlling scheme that can flip 90 % of the photocurrent by a slight change of laser frequency. For the barium atom, we computed the phase lag between 6s1/2 and 5d3/2 ionization continua, which agrees with the experimental results that a previous phenomenological model failed to reproduce. Our treatment also develops formulas to describe the effects of hyperfine depolarization on multiphoton ionization processes, and it identifies resonances that had not been observed and classified in previous experiments. <br>  </p>