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

被引:16
作者
Binz, Marcel [1 ]
Bruder, Lukas [1 ]
Chen, Lipeng [2 ]
Gelin, Maxim F. [3 ]
Domcke, Wolfgang [4 ]
Stienkemeier, Frank [1 ]
机构
[1] Univ Freiburg, Inst Phys, Hermann Herder Str 3, D-79104 Freiburg, Germany
[2] Ecole Polytech Fed Lausanne EPFL, Lab Theoret Phys Chem, Inst Sci & Ingn Chim, CH-1015 Lausanne, Switzerland
[3] Hangzhou Dianzi Univ, Sch Sci, Bldg 6, Hangzhou 310018, Peoples R China
[4] Tech Univ Munich, Dept Chem, Lichtenbergstr 4, D-85747 Garching, Germany
基金
欧洲研究理事会;
关键词
RABI OSCILLATIONS; COHERENT CONTROL; EXCITATION; DYNAMICS; SPECTRA; STATES;
D O I
10.1364/OE.396108
中图分类号
O43 [光学];
学科分类号
070207 ; 0803 ;
摘要
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. (C) 2020 Optical Society of America under the terms of the OSA Open Access Publishing Agreement
引用
收藏
页码:25806 / 25829
页数:24
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