Theory of Lineshapes in Optical-Optical Double Resonance Spectroscopy

[2604.02262] Theory of Lineshapes in Optical-Optical Double Resonance Spectroscopy Skip to main content Search Submit Donate Log in Search arXiv Press Enter to search · Advanced search Physics > Optics arXiv:2604.02262 (physics) [Submitted on 2 Apr 2026 ( v1 ), last revised 30 Jun 2026 (this version, v2)] Title: Theory of Lineshapes in Optical-Optical Double Resonance Spectroscopy Authors: Kevin K. Lehmann View a PDF of the paper titled Theory of Lineshapes in Optical-Optical Double Resonance Spectroscopy, by Kevin K. Lehmann View PDF HTML (experimental) Abstract: This paper presents lineshapes for molecular Optical-Optical Double Resonance (DR) Spectroscopy with arbitrary strength for both pump and probe field using the steady-state solutions for the 3-level density matrix. When the Doppler broadening can be neglected, the results are analytical, and the probe spectrum is a pair of Lorentzian lines that display Autler-Townes splitting, and each has an angular frequency half-width half maximum equal to the relaxation rates, which are all assumed equal. When Doppler broadening is introduced, one must resort to numerical integration except for the limit of weak pump and probe fields. When the Doppler width is assumed much larger than the pump and probe Rabi Frequencies, the calculated DR lineshapes are found to be Lorentzian with a strong pump field limit that is proportional to the pump Rabi frequency, what is commonly known as power broadening. However, the width does not equal the Rabi frequency and is different for co- and counter-propagating pump and probe fields. Furthermore, that broadening is largely inhomogeneous, despite the Lorentzian shape. The saturation power is found to be about 4 times higher than for the bare probe transition with the same relaxation rate, dramatically lower than that expected if the width is interpreted as homogeneous. Comments: 36 pages, 18 figures Subjects: Optics (physics.optics) ; Chemical Physics (physics.chem-ph) Cite as: arXiv:2604.02262 [physics.optics] (or arXiv:2604.02262v2 [physics.optics] for this version) https://doi.org/10.48550/arXiv.2604.02262 Focus to learn more arXiv-issued DOI via DataCite Journal reference: Journal of Chemical Physics 165, 064118 (2026) Related DOI : https://doi.org/10.1063/5.0336550 Focus to learn more DOI(s) linking to related resources Submission history From: Kevin K. Lehmann [ view email ] [v1] Thu, 2 Apr 2026 16:54:57 UTC (892 KB) [v2] Tue, 30 Jun 2026 20:58:49 UTC (1,053 KB) Full-text links: Access Paper: View a PDF of the paper titled Theory of Lineshapes in Optical-Optical Double Resonance Spectroscopy, by Kevin K. Lehmann View PDF HTML (experimental) TeX Source view license Current browse context: physics.optics < prev | next > new | recent | 2026-04 Change to browse by: physics physics.chem-ph References & Citations NASA ADS Google Scholar Semantic Scholar export BibTeX citation Loading... BibTeX formatted citation × loading... Data provided by: Bookmark Bibliographic Tools Bibliographic and Citation Tools Bibliographic Explorer Toggle Bibliographic Explorer ( What is the Explorer? ) Connected Papers Toggle Connected Papers ( What is Connected Papers? ) Litmaps Toggle Litmaps ( What is Litmaps? ) scite.ai Toggle scite Smart Citations ( What are Smart Citations? ) Code, Data, Media Code, Data and Media Associated with this Article alphaXiv Toggle alphaXiv ( What is alphaXiv? ) Links to Code Toggle CatalyzeX Code Finder for Papers ( What is CatalyzeX? ) DagsHub Toggle DagsHub ( What is DagsHub? ) GotitPub Toggle Gotit.pub ( What is GotitPub? ) Huggingface Toggle Hugging Face ( What is Huggingface? ) ScienceCast Toggle ScienceCast ( What is ScienceCast? ) Demos Demos Replicate Toggle Replicate ( What is Replicate? ) Spaces Toggle Hugging Face Spaces ( What is Spaces? ) Spaces Toggle TXYZ.AI ( What is TXYZ.AI? ) Related Papers Recommenders and Search Tools Link to Influence Flower Influence Flower ( What are Influence Flowers? ) Core recommender toggle CORE Recommender ( What is CORE? ) Author Venue Institution Topic About arXivLabs arXivLabs: experimental projects with community collaborators arXivLabs is a framework that allows collaborators to develop and share new arXiv features directly on our website. Both individuals and organizations that work with arXivLabs have embraced and accepted our values of openness, community, excellence, and user data privacy. arXiv is committed to these values and only works with partners that adhere to them. Have an idea for a project that will add value for arXiv's community? Learn more about arXivLabs . Which authors of this paper are endorsers? | Disable MathJax ( What is MathJax? ) We gratefully acknowledge support from our major funders , member institutions , , and all contributors. About · Help · Contact · Subscribe · Copyright · Privacy · Accessibility · Operational Status (opens in new tab) Major funding support from

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