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The effects of high pulse intensity and chirp on two-dimensional electronicspectroscopy signals are experimentally investigated in the highlynon-perturbative regime using atomic rubidium vapor as clean model system. Dataanalysis is performed based on higher-order Feynman diagrams andnon-perturbative numerical simulations of the system response. It is shown thathigher-order contributions may lead to a fundamental change of the staticappearance and beating-maps of the 2D spectra and that chirped pulses enhanceor suppress distinct higher-order pathways. We further give an estimate of thethreshold intensity beyond which the high-intensity effects become visible forthe system under consideration.

Effects of high pulse intensity and chirp in two-dimensional electronic spectroscopy of an atomic vapor