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In this article, we present a simulation study of the linear and nonlinearspectroscopy of dense atomic vapors. Motivated by recent experiments, we focuson double quantum spectroscopy which directly probes dipole-dipoleinteractions. By including explicitly thermal velocity, we show thattemperature has an important impact on the self-broadening mechanism of thelinear and nonlinear spectra. We also provide analytical expressions for theresponse functions in the short time limit using the two-body approximationwhich shows that double quantum spectroscopy for atomic vapors directly probesthe transition amplitude of the electronic excitation between two atoms. Wealso propose an expression for the double quantum spectrum that includes theeffect of Doppler broadening and we discuss the effect of density on thespectrum. We show that when Doppler broadening is negligible compared toself-broadening the double quantum spectrum scales with the atomic densitywhile when Doppler broadening dominates it scales as the square of the density.

Double-quantum spectroscopy of dense atomic vapors: interplay between Doppler and self-broadenings