Polarization-dependent Intensity Ratios in Double Resonance Spectroscopy

[2308.09828] Polarization-dependent Intensity Ratios in Double Resonance Spectroscopy Skip to main content Search Submit Donate Log in Search arXiv Press Enter to search · Advanced search Physics > Chemical Physics arXiv:2308.09828 (physics) [Submitted on 18 Aug 2023] Title: Polarization-dependent Intensity Ratios in Double Resonance Spectroscopy Authors: Kevin K. Lehmann View a PDF of the paper titled Polarization-dependent Intensity Ratios in Double Resonance Spectroscopy, by Kevin K. Lehmann View PDF HTML (experimental) Abstract: Double Resonance is a powerful method spectroscopic method that provides an unambiguous assignment of the rigorous quantum numbers of one state of a transition. However, there is often ambiguity as to the branch ($\Delta J$) of the transition. The dependence of the intensity of the double resonance signal on the relative polarization of pump and probe radiation can be used to resolve this ambiguity and has been used for this in the past. However, the published theoretical predictions for this ratio are based upon a weak (i.e. non-saturating) field approximation. In this paper, we present theoretical predictions for these intensity ratios for cases where the pump field is strongly saturating, in the two limits of transitions dominated by homogeneous and inhomogeneous broadening. While saturation, as can be expected, reduces the magnitude of the polarization effect (driving the intensity ratio closer to unity), polarization anisotropy remains even with a strongly saturating probe field in most cases. For the case of an inhomogeneously broadened line, as when Doppler broadening linewidth dominates over even the power broadened homogeneous line width, a large fraction of the low pump power anisotropy remains. Results are presented for both the case of linear and circular pump and probe field polarizations. The present predictions are compared with experimental measurements on CH$_4$ ground state $\rightarrow \nu_3 \rightarrow 3\nu_3$ transitions recently reported by de Oliveira et al and found to be in better agreement than the weak field predictions. Comments: 18 pages including 6 figures Subjects: Chemical Physics (physics.chem-ph) Cite as: arXiv:2308.09828 [physics.chem-ph] (or arXiv:2308.09828v1 [physics.chem-ph] for this version) https://doi.org/10.48550/arXiv.2308.09828 Focus to learn more arXiv-issued DOI via DataCite Journal reference: Journal of Chemical Physics 159, 184202 (2023) Related DOI : https://doi.org/10.1063/5.0172828 Focus to learn more DOI(s) linking to related resources Submission history From: Kevin K. Lehmann [ view email ] [v1] Fri, 18 Aug 2023 21:35:37 UTC (422 KB) Full-text links: Access Paper: View a PDF of the paper titled Polarization-dependent Intensity Ratios in Double Resonance Spectroscopy, by Kevin K. 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