Effects of high pulse intensity and chirp in two-dimensional electronic spectroscopy of an atomic vapor
Marcel Binz, Lukas Bruder, Lipeng Chen, Maxim F. Gelin, Wolfgang Domcke, Frank Stienkemeier
Abstract
The 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.