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arXiv:2609.28287

Decoherence Tuning in Voltage-Driven Plasmonic Cavities

Yuchen Wang, Oliver Tan, Norah M. Hoffmann

quant-phphysics.chem-phphysics.opticsSubmitted Sep 23, 2026• Announced Sep 24, 2026
arXivHTMLPDF

Abstract

Strong light-matter coupling offers a powerful framework for modifying molecular structure, dynamics, and optical response, yet achieving this regime at the single-molecule level remains a central challenge. Scanning Tunneling Microscope Break Junctions (STM-BJ) provide a promising route by combining single-molecule addressability with extreme nanoscale field confinement. However, the metallic environment that enables such confinement also introduces substantial plasmonic and excitonic losses, raising the question of how strong coupling can be realized in a metal-molecule-metal junction. Here, we identify the voltage as the key control parameter. We show that the applied bias not only drives the formation of an interfacial exciton through resonant charge transport but also suppresses its coupling to metallic loss channels. Simultaneously, the plasmonic cavity retains extreme mode confinement while the availability of modes is moderately tuned by voltage. Together, these results establish voltage-driven STM-BJs as electrically tunable single-molecule plasmonic cavities and open new routes for using the powerful STM-BJ toolbox, including quantum transport, tracking chemical dynamics, optoelectronics, and molecular-scale quantum control under strong light-matter coupling.

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Strong light-matter coupling offers a powerful framework for modifying molecular structure, dynamics, and optical response, yet achieving this regime at the single-molecule level remains a central challenge. Scanning Tunneling Microscope Break Junctions (STM-BJ) provide a promising route by combining single-molecule addressability with extreme nanoscale field confinement. However, the metallic environment that enables such confinement also introduces substantial plasmonic and excitonic losses, raising the question of how strong coupling can be realized in a metal-molecule-metal junction. Here, we identify the voltage as the key control parameter. We show that the applied bias not only drives the formation of an interfacial exciton through resonant charge transport but also suppresses its coupling to metallic loss channels. Simultaneously, the plasmonic cavity retains extreme mode confinement while the availability of modes is moderately tuned by voltage. Together, these results establish voltage-driven STM-BJs as electrically tunable single-molecule plasmonic cavities and open new routes for using the powerful STM-BJ toolbox, including quantum transport, tracking chemical dynamics, optoelectronics, and molecular-scale quantum control under strong light-matter coupling.
Recent scanning tunneling microscopy (STM) experiments reported single-molecule fluorescence induced by tunneling currents in the nanoplasmonic cavity formed by the STM tip and the substrate. The electric field of the cavity mode couples with the current-induced charge fluctuations of the molecule, allowing the excitation of photons. We investigate theoretically this system for the experimentally relevant limit of large damping rate κ for the cavity mode and arbitrary coupling strength to a single-electronic level. We find that for bias voltages close to the first inelastic threshold of photon emission, the emitted light displays antibunching behavior with vanishing second-order photon correlation function. At the same time, the current and the intensity of emitted light display Franck-Condon steps at multiples of the cavity frequency ω_{c} with a width controlled by κ rather than the temperature T. For large bias voltages, we predict strong photon bunching of the order of κ/Γ where Γ is the electronic tunneling rate. Our theory thus predicts that strong coupling to a single level allows current-driven nonclassical light emission.
Scanning tunneling microscope (STM)-induced luminescence provides an ideal platform for electrical generation and the atomic-scale manipulation of nonclassical states of light. However, despite its extreme importance in quantum technologies, squeezed light emission with reduced quantum fluctuations has hitherto not been demonstrated in such a platform. Here, we theoretically predict that the emitted light from the plasmon mode can be squeezed in an STM single molecular junction subject to an external laser drive. Going beyond the traditional paradigm that generates squeezing with the quadratic interaction of photons, our prediction explores the molecular coherence involved in an anharmonic energy spectrum of a coupled plasmon-molecule-exciton system. Furthermore, we show that, by selectively exciting the energy ladder, the squeezed plasmon can show either sub- or super-Poissonian statistical properties. We also demonstrate that, following the same principle, the molecular excitonic mode can be squeezed simultaneously.
Abstract In the light–matter strong coupling regime, the excited state of quantum emitters is inextricably linked to a photonic mode, leading to hybrid states that are part light and part matter. Recently, there has been a huge effort to realize strong coupling with nanoplasmonics, since it provides a versatile environment to study and control molecules in ambient conditions. Among the most promising designs are plasmonic nanocavities that confine light to unprecedentedly small volumes. Such nanocavities, though, support multiple types of modes, with different field profiles and radiative decay rates (bright and dark modes). Here, we show theoretically that the different nature of these modes leads to mode beating within the nanocavity and the Rabi oscillations, which alters the spatiotemporal dynamics of the hybrid system. By specifically designing the illumination setup, we decompose and control the dark and bright plasmon mode excitation and therefore their coupling with quantum emitters. Hence, this work opens new routes for dynamically dressing emitters, to tailor their hybrid states with external radiation.
Abstract Quantum nanophotonics places nanoscale structuring in direct dialogue with photonic quantum information—compressing functionality to the few-nanometre, few-femtosecond frontier while retaining energy efficiency, speed and room-temperature operation. We highlight nanoplasmonic cavity-QED architectures in which extreme mode confinement delivers strong coupling under ambient conditions, enabling ultrafast single-photon emission and near-field multipartite entanglement using industry-grade near-field transducers that nanofocus guided light at practical efficiencies. We set these advances against the arc from early plasmonic cQED proposals and single-emitter Purcell studies to modern time-domain measurements that resolve sub-picosecond polariton/Rabi dynamics—establishing a clear route from concept to device. In parallel, we point to low-loss, high-index Mie resonators whose spectrally sharp electric and magnetic modes afford narrow-band coherent control, filtering and radiation-pattern engineering, and which naturally co-integrate in hybrid metal–dielectric stacks that combine ultrastrong local coupling with low-loss routing and storage. Finally, we discuss quantum nanoplasmonic coherent perfect absorption (qnCPA)—a waveguide-fed, non-perturbing protocol that selectively prepares and protects plasmon–emitter dressed states via dissipation-assisted, unidirectional feeding. Together with macroscopic QED and quantum quasinormal-mode quantization, which regularize open, lossy resonators and clarify when loss can be a resource, these developments chart robust, chip-scale routes to room-temperature quantum technologies.
The coherent interaction between quantum emitters and photonic modes in cavities underlies many of the current strategies aiming at generating and controlling photonic quantum states. A plasmonic nanocavity provides a powerful solution for reducing the effective mode volumes down to nanometre scale, but spatial control at the atomic scale of the coupling with a single molecular emitter is challenging. Here we demonstrate sub-nanometre spatial control over the coherent coupling between a single molecule and a plasmonic nanocavity in close proximity by monitoring the evolution of Fano lineshapes and photonic Lamb shifts in tunnelling electron-induced luminescence spectra. The evolution of the Fano dips allows the determination of the effective interaction distance of ∼1 nm, coupling strengths reaching ∼15 meV and a giant self-interaction induced photonic Lamb shift of up to ∼3 meV. These results open new pathways to control quantum interference and field-matter interaction at the nanoscale.
The quantum control of emitters is a key issue for quantum information processing at the nanoscale. This generally necessitates the strong coupling of emitters to a high Q-cavity for efficient manipulation of the atoms and field dynamics (cavity quantum electrodynamics or cQED). Since almost a decade, strong efforts are put to transpose cQED concepts to plasmonics in order to profit of the strong mode confinement of surface plasmons polaritons. Despite the intrinsic presence of lossy channels leading to strong decoherence in plasmonics systems, it has been experimentally proven that it is possible to reach the strong coupling regim [1].