Binz, MarcelBruder, LukasChen, LipengGelin, Maxim F.Domcke, WolfgangStienkemeier, Frank2020-09-172020-09-172020-09-172020-08-3110.1364/OE.396108https://infoscience.epfl.ch/handle/20.500.14299/171744WOS:000565713200012The effects of high pulse intensity and chirp on two-dimensional electronic spectroscopy signals are experimentally investigated in the highly non-perturbative regime using atomic rubidium vapor as clean model system. Data analysis is performed based on higher-order Feynman diagrams and non-perturbative numerical simulations of the system response. It is shown that higher-order contributions may lead to a fundamental change of the static appearance and beating-maps of the 2D spectra and that chirped pulses enhance or suppress distinct higher-order pathways. We further give an estimate of the threshold intensity beyond which the high-intensity effects become visible for the system under consideration. (C) 2020 Optical Society of America under the terms of the OSA Open Access Publishing AgreementOpticsrabi oscillationscoherent controlexcitationdynamicsspectrastatestext::journal::journal article::research article