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Unexpected two-quantum resonances are observed in potassium vapor using two-dimensional Fourier-transform spectroscopy. These transitions are an unambiguous indication of many-body interactions, which arise from the long-range interatomic coupling that is responsible for resonance self-broadening.
Two-dimensional Fourier-transform spectroscopy shows a strong variation in the biexciton binding energy across the inhomogeneous absorption width. This effect is observed for both co- and cross-linearly polarized excitation, where the latter suppresses many-body interactions.
Using a one-dimensional tight-binding model which contains the correct selection rules we compute 2DFTS in the coherent x(3)-limit. By comparing theoretical spectra resulting from different orders in the Coulomb interaction we can clearly identify the influence of the many-particle interaction on the various signatures that are visible in the spectrograms.
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