Effect of pulse propagation on the two-dimensional photon echo spectrum of multilevel systems

The effect of pulse propagation on the two-dimensional photon echo (2DPE) spectrum of multilevel systems is investigated using a perturbative method. At high optical densities (OD) peak profiles are broadened asymmetrically, in most cases more strongly along the omega(2) direction than along the omega(1) direction. The amount of broadening is determined both by the OD and by the dynamics of the system. In addition, especially if the different transitions in the system are of unequal strength, the relative intensity of the peaks changes with OD. But even if the transition strengths are the same, the behavior of the cross peaks is different from the diagonal peaks. Since peak shape and relative intensity are important parameters in the interpretation of 2DPE spectra, such OD effects should be taken into account. (C) 2003 American Institute of Physics.