Coherent state sampling for molecular vibronic spectra

Coherent state sampling for molecular vibronic spectra | Research Square window.SnipcartSettings = { analytics: { enabled: false } }; (function() { var accessVector = localStorage.getItem('access_vector') || ''; window.dataLayer = window.dataLayer || []; if (accessVector) { window.dataLayer.push({ user: { profile: { profileInfo: { snid: accessVector } } } }); } })(); (function(w,d,s,l,i){w[l]=w[l]||[];w[l].push({'gtm.start':new Date().getTime(),event:'gtm.js'});var f=d.getElementsByTagName(s)[0],j=d.createElement(s),dl=l!='dataLayer'?'&l='+l:'';j.async=true;j.src='https://www.googletagmanager.com/gtm.js?id='+i+dl;f.parentNode.insertBefore(j,f);})(window,document,'script','dataLayer','GTM-K279D39R'); Browse Preprints In Review Journals COVID-19 Preprints AJE Video Bytes Research Tools Research Promotion AJE Professional Editing AJE Rubriq About Preprint Platform In Review Editorial Policies Our Team Advisory Board Help Center Sign In Submit a Preprint Cite Share Download PDF Article Coherent state sampling for molecular vibronic spectra Iurii Konyshev, Ravi Pradip, Oliver Page, Caghan Ünlüer, Rinat T. Nasibullin, and 3 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-8593810/v1 This work is licensed under a CC BY 4.0 License Status: Under Review Version 1 posted 8 You are reading this latest preprint version Abstract Electronic spectroscopy is today among the most powerful methods for studying chemical systems, and state-resolved (line-assigned) simulations are essential for attributing spectral features to specific vibrational excitations. The standard time-independent sum-over-states (SOS) route provides line assignments; while effective with truncation and prescreening, it can become computationally demanding as the number of modes increases. Vibronic boson sampling (VBS) offers an event-based alternative, but scaling photonic implementations remains challenging and the required vibronic inputs can be demanding for larger systems. Here we introduce coherent-state sampling (CSS), a sampling scheme for the Linear Coupling Model (LCM), where vibrational modes are independent. This enables a photonic architecture based on a single reconfigurable optical channel with essentially fixed hardware complexity; increasing system size is handled by additional measurement iterations rather than additional optical modes. Using pentacene as a test case, we demonstrate an end-to-end workflow—electronic-structure input, sampling strategy, hardware validation, and comparison to experiment—showing that both a laptop implementation and a superconducting-detector photonic implementation reproduce reference spectra with high fidelity and yield band shapes in good agreement with experiment. While not targeting quantum advantage, CSS provides a practically scalable, state-resolved tool for LCM vibronic spectroscopy and a controlled displacement-dominated complement to more general VBS schemes. Physical sciences/Optics and photonics Physical sciences/Physics Full Text Additional Declarations No competing interests reported. Cite Share Download PDF Status: Under Review Version 1 posted Reviews received at journal 19 Mar, 2026 Reviewers agreed at journal 02 Mar, 2026 Reviewers agreed at journal 12 Feb, 2026 Reviewers invited by journal 11 Feb, 2026 Editor assigned by journal 29 Jan, 2026 Editor invited by journal 28 Jan, 2026 Submission checks completed at journal 27 Jan, 2026 First submitted to journal 27 Jan, 2026 You are reading this latest preprint version Research Square lets you share your work early, gain feedback from the community, and start making changes to your manuscript prior to peer review in a journal. As a division of Research Square Company, we’re committed to making research communication faster, fairer, and more useful. We do this by developing innovative software and high quality services for the global research community. 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Also discoverable on Platform About Our Team In Review Editorial Policies Advisory Board Help Center Resources Author Services Accessibility API Access RSS feed Manage Cookie Preferences © Research Square 2026 | ISSN 2693-5015 (online) Privacy Policy Terms of Service Do Not Sell My Personal Information {"props":{"pageProps":{"initialData":{"identity":"rs-8593810","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":591153624,"identity":"cf3bc465-5472-4b2f-825c-709e2b1e890d","order_by":0,"name":"Iurii Konyshev","email":"","orcid":"","institution":"University of Heidelberg","correspondingAuthor":false,"prefix":"","firstName":"Iurii","middleName":"","lastName":"Konyshev","suffix":""},{"id":591153625,"identity":"ff7344d6-7149-4019-9b6a-dbde248d42fb","order_by":1,"name":"Ravi Pradip","email":"","orcid":"","institution":"University of Heidelberg","correspondingAuthor":false,"prefix":"","firstName":"Ravi","middleName":"","lastName":"Pradip","suffix":""},{"id":591153626,"identity":"090db81f-1f56-4c97-b6df-ca6e093ab14b","order_by":2,"name":"Oliver Page","email":"","orcid":"","institution":"University of Heidelberg","correspondingAuthor":false,"prefix":"","firstName":"Oliver","middleName":"","lastName":"Page","suffix":""},{"id":591153627,"identity":"f2e3dd94-e37e-4187-83d6-70be4eeb5f38","order_by":3,"name":"Caghan Ünlüer","email":"","orcid":"","institution":"University of Heidelberg","correspondingAuthor":false,"prefix":"","firstName":"Caghan","middleName":"","lastName":"Ünlüer","suffix":""},{"id":591153628,"identity":"f0126656-2cd0-4a61-9ced-0a7717b63f1a","order_by":4,"name":"Rinat T. 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The standard time-independent sum-over-states (SOS) route provides line assignments; while effective with truncation and prescreening, it can become computationally demanding as the number of modes increases. Vibronic boson sampling (VBS) offers an event-based alternative, but scaling photonic implementations remains challenging and the required vibronic inputs can be demanding for larger systems. Here we introduce coherent-state sampling (CSS), a sampling scheme for the Linear Coupling Model (LCM), where vibrational modes are independent. This enables a photonic architecture based on a single reconfigurable optical channel with essentially fixed hardware complexity; increasing system size is handled by additional measurement iterations rather than additional optical modes. 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