2024/11/20 by Rishabh Tripathi, Tripathi, Rishabh, Maurya, Krishna K. +5 · 1 citation
Biochemistry, Genetics and Molecular Biology · Physics and Astronomy · #Advanced Fiber Laser Technologies #Advanced Optical Sensing Technologies #Computational Physics (physics.comp-ph) #FOS: Physical sciences #Optics (physics.optics) #Spectroscopy Techniques in Biomedical and Chemical Research
paper · pdf · doi:10.48550/arxiv.2411.13290
openalex publication_date 2024/11/20 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/28
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 δ-function in time. Here, we use the phase-cycling method for 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. Additionally, 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 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.