Simulating Optical Coherent Nonlinear Response for High-Intensity Excitation

Calculation of the coherent nonlinear response of a system is essential to correctly interpret results from advanced techniques such as two-dimensional coherent spectroscopy (2DCS). Usually, even for the simplest systems, such calculations are either performed for low-intensity excitations where perturbative methods are valid and/or by assuming a simplified pulse envelope, such as a {\delta}-function in time. We present exact calculations using the phase-cycling method without making the aforementioned approximations. We introduce a generalized version of the phase-cycling method to isolate an arbitrary N-wave mixing signal. We then apply this method to model the saturation of the nonlinear signal from excitons in semiconductor quantum wells, which is consistent with 2DCS experiments. We also present simulation results that replicate previously-reported experiments with high-intensity excitation of semiconductor quantum dots. By accurately reproducing a variety of phenomena such as higher-order contributions, switching of coherent signal, and changes in photon-echo transients, we prove the efficacy of the phase-cycling method to calculate the coherent nonlinear signal for high-intensity excitation. This method would be particularly useful for systems with multiple, well-separated peaks and/or large inhomogeneity.