Nonresonant coherent two-dimensional spectroscopy

0560632 - FZÚ 2023 RIV NL eng J - Journal Article
Dostál, Jakub
Nonresonant coherent two-dimensional spectroscopy.
Spectrochimica Acta Part A-Molecular and Biomolecular Spectroscopy. Roč. 267, FEB (2022), č. článku 120441. ISSN 1386-1425. E-ISSN 1873-3557
R&D Projects: GA MŠMT EF16_019/0000789; GA MŠMT EF15_003/0000447
Grant - others:OP VVV - ADONIS(XE) CZ.02.1.01/0.0/0.0/16_019/0000789; OP VVV - ELIBIO(XE) CZ.02.1.01/0.0/0.0/15_003/0000447
Institutional support: RVO:68378271
Keywords : coherent two-dimensional spectroscopy * nonresonant interaction * optical Kerr effect * stimulated Raman scattering * two-photon absorption * cross-phase modulation
OECD category: Atomic, molecular and chemical physics (physics of atoms and molecules including collision, interaction with radiation, magnetic resonances, Mössbauer effect)
Impact factor: 4.4, year: 2022
Method of publishing: Limited access
https://doi.org/10.1016/j.saa.2021.120441

Coherent electronic two-dimensional spectroscopy is nowadays a matured experimental technique that monitors the time evolution of the studied sample after its resonant optical excitation. However, the experimental experience shows that even nonresonant interactions can provide detectable spectral contributions. These are often present as a weak parasitic signals originating in the solvent and/or cuvette walls underlying the resonant spectrum of the actual sample and as such they are usually discarded from the analysis. In this work, we adapt the formalism of double-sided Feynman diagrams for the needs of coherent two-dimensional spectroscopy in the nonresonant regime. We analytically calculate the third-order polarization of a two-level and several variants of three-level systems. As a result, we demonstrate the typical appearance of the optical Kerr-effect, cross-phase modulation, excited-state coherence, two-photon absorption and stimulated Raman scattering in the 2D spectrum.
Permanent Link: https://hdl.handle.net/11104/0333524