Multidimensional semiclassical single- and double-quantum spectroscopy of anharmonic molecular polaritons
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Quantum Physics arXiv:2604.21158 (quant-ph) [Submitted on 22 Apr 2026] Title:Multidimensional semiclassical single- and double-quantum spectroscopy of anharmonic molecular polaritons Authors:Michael Reitz, Harsh Bhakta, Wei Xiong, Joel Yuen-Zhou View a PDF of the paper titled Multidimensional semiclassical single- and double-quantum spectroscopy of anharmonic molecular polaritons, by Michael Reitz and 3 other authors View PDF HTML (experimental) Abstract:We present a general and efficient approach to compute phase-resolved multidimensional spectra of anharmonic molecular polaritons, based on a semiclassical evolution of the molecular Hamiltonian and cavity field in the large-$\mathcal{N}$ limit of many molecules coupled to a confined photonic mode. By systematically expanding the response in both amplitudes and phases of the input fields, our method enables a transparent and computationally simple construction of phase-cycled two-dimensional single- and double-quantum polariton spectra from the underlying nonlinear signal components. Here, phase cycling acts as an analogue of phase matching with oblique pulses, allowing for the isolation of the contributing nonlinear pathways in Liouville space. We specialize to vibrational polaritons and benchmark the method through direct comparison with experimentally measured single-quantum spectra, providing an explanation for the longstanding puzzle of the polariton bleach effect observed at short waiting times. Further, we show how the imprint of various types of anharmonicities on the double-excitation manifold can be directly probed and analyzed through double-quantum coherence spectroscopy. Taken together, our results establish a practical and powerful framework for the modeling and interpretation of nonlinear spectroscopic experiments on strongly coupled light-matter platforms and for guiding the design of cavity-enhanced molecular platforms. Comments: Subjects: Quantum Physics (quant-ph); Mesoscale and Nanoscale Physics (cond-mat.mes-hall); Chemical Physics (physics.chem-ph); Optics (physics.optics) Cite as: arXiv:2604.21158 [quant-ph] (or arXiv:2604.21158v1 [quant-ph] for this version) https://doi.org/10.48550/arXiv.2604.21158 Focus to learn more arXiv-issued DOI via DataCite (pending registration) Submission history From: Michael Reitz [view email] [v1] Wed, 22 Apr 2026 23:54:15 UTC (4,624 KB) Full-text links: Access Paper: View a PDF of the paper titled Multidimensional semiclassical single- and double-quantum spectroscopy of anharmonic molecular polaritons, by Michael Reitz and 3 other authorsView PDFHTML (experimental)TeX Source view license Ancillary-file links: Ancillary files (details): dqc_movie.gif Current browse context: quant-ph new | recent | 2026-04 Change to browse by: cond-mat cond-mat.mes-hall physics physics.chem-ph physics.optics References & Citations INSPIRE HEP NASA ADSGoogle 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?)