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.
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14 March 2025
Research Article|
March 18 2025
Coherent nonlinear optical response for high-intensity excitation
Special Collection:
David Jonas Festschrift
Rishabh Tripathi
;
Rishabh Tripathi
(Conceptualization, Data curation, Formal analysis, Investigation, Software, Validation, Visualization, Writing – original draft, Writing – review & editing)
Department of Physics, Indian Institute of Science Education and Research Bhopal
, Bhopal 462066, India
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Krishna K. Maurya
;
Krishna K. Maurya
(Data curation, Software, Visualization, Writing – review & editing)
Department of Physics, Indian Institute of Science Education and Research Bhopal
, Bhopal 462066, India
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Pradeep Kumar
;
Pradeep Kumar
(Data curation, Software, Visualization)
Department of Physics, Indian Institute of Science Education and Research Bhopal
, Bhopal 462066, India
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Bhaskar De
;
Bhaskar De
(Data curation, Software, Visualization)
Department of Physics, Indian Institute of Science Education and Research Bhopal
, Bhopal 462066, India
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Rohan Singh
Rohan Singh
a)
(Conceptualization, Data curation, Funding acquisition, Investigation, Methodology, Project administration, Software, Supervision, Validation, Visualization, Writing – original draft, Writing – review & editing)
Department of Physics, Indian Institute of Science Education and Research Bhopal
, Bhopal 462066, India
a)Author to whom correspondence should be addressed: [email protected]
Search for other works by this author on:
Rishabh Tripathi
Krishna K. Maurya
Pradeep Kumar
Bhaskar De
Rohan Singh
a)
Department of Physics, Indian Institute of Science Education and Research Bhopal
, Bhopal 462066, India
a)Author to whom correspondence should be addressed: [email protected]
J. Chem. Phys. 162, 114111 (2025)
Article history
Received:
November 20 2024
Accepted:
February 20 2025
Citation
Rishabh Tripathi, Krishna K. Maurya, Pradeep Kumar, Bhaskar De, Rohan Singh; Coherent nonlinear optical response for high-intensity excitation. J. Chem. Phys. 14 March 2025; 162 (11): 114111. https://doi.org/10.1063/5.0249809
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