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

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-perturba...

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Bibliographic Details
Published inOptics express Vol. 28; no. 18; pp. 25806 - 25829
Main Authors Binz, Marcel, Bruder, Lukas, Chen, Lipeng, Gelin, Maxim F., Domcke, Wolfgang, Stienkemeier, Frank
Format Journal Article
LanguageEnglish
Published 31.08.2020
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Summary: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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ISSN:1094-4087
1094-4087
DOI:10.1364/OE.396108