One- and two-photon ionization cross sections of the laser excited 6s6p¹P₁ state of barium

Stimulated by a recent measurement of coherent control in photoionization of atomic barium, we have calculated one- and two-photon ionization cross sections of the aligned 6s6p^1P_1 state of barium in the energy range between the 5d_{3/2} and 5d_{5/2} states of Ba^+. We have also measured these photionization spectra in the same energy region, driving the one- or two-photon processes with the second or first harmonic of a tunable dye laser, respectively. Our calculations employ the eigenchannel R-matrix method and multichannel quantum defect theory to calculate the rich array of autoionizing resonances in this energy range. The non-resonant two-photon process is described using lowest-order perturbation theory for the photon-atom interactions, with a discretized intermediate state one-electron continuum. The calculations provide an absolute normalization for the experiment, and they accurately reproduce the rich resonance structures in both the one and two-photon cross sections, and confirm other aspects of experimental observations. These results demonstrate the ability of these computationally inexpensive methods to reproduce the experimental observables in one- and two-photon ionization of heavy alkaline earths, and they lay the groundwork for future studies of the phase-controlled interference between one-photon and two-photon ionization processes.