We investigate two-frequency photoassociation of a weakly bound molecular
state, focusing on a regime where the ac Stark shift is comparable to the
halo-state energy. In this "high-intensity" regime, we observe features absent
in low-intensity two-frequency photoassociation. We experimentally measure the
spectra of 86Sr atoms coupled to the least bound state of the
86Sr2​ ground electronic channel through an intermediate electronically
excited molecular state. We compare the spectra to a simple three-level model
that includes a two-frequency drive on each leg of the transition. With
numerical solution of the time-dependent Schrodinger equation, we show that
this model accurately captures (1) the existence of experimentally observed
satellite peaks that arise from nonlinear processes, (2) the locations of the
two-photon peak in the spectrum, including ac Stark shifts, and (3) in some
cases, spectral lineshapes. To better understand these numerical results, we
develop an approximate treatment of this model, based on Floquet and
perturbation theory, that gives simple formulas that accurately capture the
halo-state energies. We expect these expressions to be valuable tools to
analyze and guide future two-frequency photoassociation experiments.Comment: 12 pages, 7 figure