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@article{Bressan:2021:10.1063/5.0051435,
author = {Bressan, G and van, Thor JJ},
doi = {10.1063/5.0051435},
journal = {The Journal of Chemical Physics},
pages = {1--10},
title = {Theory of two-dimensional spectroscopy with intense laser fields},
url = {http://dx.doi.org/10.1063/5.0051435},
volume = {154},
year = {2021}
}

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TY  - JOUR
AB  - Two-dimensional vibrational and electronic spectroscopic observables of isotropically oriented molecular samples in solution are sensitive to laser field intensities and polarization. The third-order response function formalism predicts a signal that grows linearly with the field strength of each laser pulse, thus lacking a way of accounting for non-trivial intensity-dependent effects, such as saturation and finite bleaching. An analytical expression to describe the orientational part of the molecular response, which, in the weak-field limit, becomes equivalent to a four-point correlation function, is presented. Such an expression is evaluated for Liouville-space pathways accounting for diagonal and cross peaks for all-parallel and cross-polarized pulse sequences, in both the weak- and strong-field conditions, via truncation of a Taylor series expansion at different orders. The results obtained in the strong-field conditions suggest how a careful analysis of two-dimensional spectroscopic experimental data should include laser pulse intensity considerations when determining molecular internal coordinates.
AU  - Bressan,G
AU  - van,Thor JJ
DO  - 10.1063/5.0051435
EP  - 10
PY  - 2021///
SN  - 0021-9606
SP  - 1
TI  - Theory of two-dimensional spectroscopy with intense laser fields
T2  - The Journal of Chemical Physics
UR  - http://dx.doi.org/10.1063/5.0051435
UR  - https://aip.scitation.org/doi/10.1063/5.0051435
UR  - http://hdl.handle.net/10044/1/89993
VL  - 154
ER  -

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ProfessorJaspervan Thor

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