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This research establishes steady-state electrical current as a direct probe for strong light-matter coupling in single-molecule junctions, offering a new method to detect polaritonic states without relying solely on optical spectroscopy. By validating this signature against environmental noise and nuclear motion, the study provides a robust framework for controlling molecular dynamics at the nanoscale through quantum transport signatures.
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Steady--State Current Signatures of Strong Light--Matter Coupling in Single--Molecule Junctions

arXiv2 min read

arXiv:2609.31265v1 Announce Type: new Abstract: Strong light-matter coupling offers exciting opportunities for controlling molecular properties, yet resolving single-molecule behavior from collective effects remains a challenge. Recent experiments in scanning tunneling microscope break junctions (STM-BJs) have demonstrated strong light-matter coupling at the single-molecule level. Because STM-BJs provide direct access to molecular-junction currents, we investigate whether strong coupling leaves a measurable fingerprint in transport, potentially probing polaritonic states beyond optical spectroscopy. Using a semiclassical mapping approach for nonequilibrium quantum transport, we find that steady-state current indeed carries a direct signature of single-molecule strong coupling. We test the robustness of this signature against electrode connectivity, nuclear motion, spatially structured electromagnetic modes, and solvent effects. While environmental factors and nuclear motion reshape the signature, the current is not a passive response but is actively influenced by coupled molecular dynamics. Our work establishes current as a tool to interpret and control strong light-matter interactions in nanoscale junctions.

Abstract:Strong light-matter coupling offers exciting opportunities for controlling molecular properties, yet resolving single-molecule behavior from collective effects remains a challenge. Recent experiments in scanning tunneling microscope break junctions (STM-BJs) have demonstrated strong light-matter coupling at the single-molecule level. Because STM-BJs provide direct access to molecular-junction currents, we investigate whether strong coupling leaves a measurable fingerprint in transport, potentially probing polaritonic states beyond optical spectroscopy. Using a semiclassical mapping approach for nonequilibrium quantum transport, we find that steady-state current indeed carries a direct signature of single-molecule strong coupling. We test the robustness of this signature against electrode connectivity, nuclear motion, spatially structured electromagnetic modes, and solvent effects. While environmental factors and nuclear motion reshape the signature, the current is not a passive response but is actively influenced by coupled molecular dynamics. Our work establishes current as a tool to interpret and control strong light-matter interactions in nanoscale junctions.

Quantum Physics (quant-ph); Mesoscale and Nanoscale Physics (cond-mat.mes-hall)

arXiv:2609.31265 [quant-ph]

(or arXiv:2609.31265v1 [quant-ph] for this version)

https://doi.org/10.48550/arXiv.2609.31265 Focus to learn more arXiv-issued DOI via DataCite (pending registration)

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Full text under the publisher's open licence · 246 words

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