Coherent Nonlinear Optical Response for High-Intensity Excitation
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arXiv
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| Autores principales: | , , , , |
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| Formato: | Preprint |
| Publicado: |
2024
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| _version_ | 1866918133790408704 |
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| author | Tripathi, Rishabh Maurya, Krishna K. Kumar, Pradeep De, Bhaskar Singh, Rohan |
| author_facet | Tripathi, Rishabh Maurya, Krishna K. Kumar, Pradeep De, Bhaskar Singh, Rohan |
| contents | 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. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2411_13290 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | Coherent Nonlinear Optical Response for High-Intensity Excitation Tripathi, Rishabh Maurya, Krishna K. Kumar, Pradeep De, Bhaskar Singh, Rohan Optics Computational Physics 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. |
| title | Coherent Nonlinear Optical Response for High-Intensity Excitation |
| topic | Optics Computational Physics |
| url | https://arxiv.org/abs/2411.13290 |