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arXiv:2411.13290 · The Journal of Chemical Physics

Coherent nonlinear optical response for high-intensity excitation

Rishabh Tripathi, Krishna K. Maurya, Pradeep Kumar, Bhaskar De, Rohan Singh

Published Mar 18, 2025• 6 citations

Abstract

The calculation of the coherent nonlinear response of a system is essential to correctly interpret results from advanced techniques such as two-dimensional coherent spectroscopy. 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 δ-function in time. Here, we use the phase-cycling method for the exact calculation of the nonlinear response without making the aforementioned approximations even for high-intensity excitation. We compare the simulation results to several experimental observations to prove the validity of these calculations. The saturation of the photon-echo signal from excitons in a semiconductor quantum well sample is measured. The excitation-intensity dependent measurement shows nonlinear contributions up to twelfth order. Intensity-dependent simulations reproduce this effect without explicitly considering higher-order interactions. In addition, we 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 signals, 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 inhomogeneities.

DOI: 10.1063/5.0249809

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