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arXiv · 2004.13366

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
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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.

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Marcel Binz, Lukas Bruder, Lipeng Chen, Maxim F. Gelin, Wolfgang Domcke, Frank Stienkemeier. 2020-04-28. Effects of high pulse intensity and chirp in two-dimensional electronic spectroscopy of an atomic vapor. https://doi.org/10.1364/oe.396108

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