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Two-dimensional electronic spectroscopy (2DES) can be implemented withdifferent geometries, e.g., BOXCARS, collinear and pump-probe geometries. Thepump-probe geometry has its advantage of overlapping only two beams andreducing phase cycling steps. However, its applications are typically limitedto observe the dynamics with single-quantum coherence and population, leavingthe challenge to measure the dynamics of the double-quantum (2Q) coherence,which reflects the many-body interactions. We propose an experimental techniquein 2DES under pump-probe geometry with a designed pulse sequence and the signalprocessing method to extract 2Q coherence. In the designed pulse sequence withthe probe pulse arriving earlier than pump pulses, our measured signal includesthe 2Q signal as well as the zero-quantum (0Q) signal. With phase cycling andthe data processing using causality enforcement, we extract the 2Q signal. Theproposal is demonstrated with the rubidium atoms. And we observe the collectiveresonances of two-body dipole-dipole interactions of both $D_{1}$ and $D_{2}$lines.

Extracting double-quantum coherence in two-dimensional electronic spectroscopy under pump-probe geometry