Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

arXiv:1907.11269 · Physical Review Letters

Single-Photon Emission Mediated by Single-Electron Tunneling in Plasmonic Nanojunctions

Q. Schaeverbeke, Rémi Avriller, Thomas Frederiksen, F. Pistolesi

Published Dec 12, 2019• 29 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1103/physrevlett.123.246601

Related papers

Plasmon Squeezing in Single-Molecule Junctions

Lei‐Lei Nian, Tao Wang, Jing‐Tao Lü

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.

Nano Letters•Nov 30, 2022•4 citations

Decoherence Tuning in Voltage-Driven Plasmonic Cavities

Yuchen Wang, Oliver Tan, Norah M. Hoffmann

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.

quant-pharXiv:2609.28287•Sep 24, 2026

Nonclassical light generation by Coulomb blockade of resonant tunneling

Ataç İmamoğlu, Y. Yamamoto

We show that the Coulomb blockade of resonant tunneling in semiconductor heterojunctions creates correlations between single-charge tunneling and single-photon emission events. When driven by a constant-current source, a mesoscopic p-i-i-i-n junction generates a regulated single-photon stream by single-electron-to-single-photon conversion. Under constant-voltage operation, the photon stream generated by the junction is antibunched and sub-Poissonian. The single-electron charging energy of the heterostructure has to exceed the width of the resonant subband and the characteristic energy of the thermal fluctuations for these correlations to be observable.

Physical review. B, Condensed matter•Dec 15, 1992•30 citations

Electrically Driven Single-Photon Superradiance from Molecular Chains in a Plasmonic Nanocavity

Yang Luo, Chen Gong, Yang Zhang +11 more

We demonstrate single-photon superradiance from artificially constructed nonbonded zinc-phthalocyanine molecular chains of up to 12 molecules. We excite the system via electron tunneling in a plasmonic nanocavity and quantitatively investigate the interaction of the localized plasmon with single-exciton superradiant states resulting from dipole-dipole coupling. Dumbbell-like patterns obtained by subnanometer resolved spectroscopic imaging disclose the coherent nature of the coupling associated with superradiant states while second-order photon correlation measurements demonstrate single-photon emission. The combination of spatially resolved spectral measurements with theoretical considerations reveals that nanocavity plasmons dramatically modify the linewidth and intensity of emission from the molecular chains, but they do not dictate the intrinsic coherence of the superradiant states. Our studies shed light on the optical properties of molecular collective states and their interaction with nanoscopically localized plasmons.

Physical Review Letters•Jun 12, 2019•91 citations

Quantum electrodynamics at room temperature coupling a single vibrating molecule with a plasmonic nanocavity

Oluwafemi Stephen Ojambati, Rohit Chikkaraddy, William Deacon +5 more

Abstract Interactions between a single emitter and cavity provide the archetypical system for fundamental quantum electrodynamics. Here we show that a single molecule of Atto647 aligned using DNA origami interacts coherently with a sub-wavelength plasmonic nanocavity, approaching the cooperative regime even at room temperature. Power-dependent pulsed excitation reveals Rabi oscillations, arising from the coupling of the oscillating electric field between the ground and excited states. The observed single-molecule fluorescent emission is split into two modes resulting from anti-crossing with the plasmonic mode, indicating the molecule is strongly coupled to the cavity. The second-order correlation function of the photon emission statistics is found to be pump wavelength dependent, varying from g (2) (0) = 0.4 to 1.45, highlighting the influence of vibrational relaxation on the Jaynes-Cummings ladder. Our results show that cavity quantum electrodynamic effects can be observed in molecular systems at ambient conditions, opening significant potential for device applications.

Nature Communications•Mar 5, 2019•174 citations

Effective Control of Photon Statistics from Electroluminescence by Fano-like Interference Effect

Lei‐Lei Nian, Tao Wang, Zu-Quan Zhang +2 more

The photon blockade induced by optical nonlinearity has been widely used to generate single-photon emission under optical driving in quantum optics. However, the same approach is difficult to achieve in electrically driven molecular junctions. Here we propose a scheme for tuning photon statistics via Fano-like interference effect in a system consisting of two molecules within one optical cavity. Under electrical pumping, a transition from photon bunching to antibunching takes place as a manifestation of the Fano-like interference. This effect persists even in the presence of the dipole-dipole interaction between molecules based on the parameters extracted from the experiments. Our proposal can be realized in current-carrying scanning tunneling microscope junctions.

The Journal of Physical Chemistry Letters•Sep 30, 2020•9 citations
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.
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.
We show that the Coulomb blockade of resonant tunneling in semiconductor heterojunctions creates correlations between single-charge tunneling and single-photon emission events. When driven by a constant-current source, a mesoscopic p-i-i-i-n junction generates a regulated single-photon stream by single-electron-to-single-photon conversion. Under constant-voltage operation, the photon stream generated by the junction is antibunched and sub-Poissonian. The single-electron charging energy of the heterostructure has to exceed the width of the resonant subband and the characteristic energy of the thermal fluctuations for these correlations to be observable.
We demonstrate single-photon superradiance from artificially constructed nonbonded zinc-phthalocyanine molecular chains of up to 12 molecules. We excite the system via electron tunneling in a plasmonic nanocavity and quantitatively investigate the interaction of the localized plasmon with single-exciton superradiant states resulting from dipole-dipole coupling. Dumbbell-like patterns obtained by subnanometer resolved spectroscopic imaging disclose the coherent nature of the coupling associated with superradiant states while second-order photon correlation measurements demonstrate single-photon emission. The combination of spatially resolved spectral measurements with theoretical considerations reveals that nanocavity plasmons dramatically modify the linewidth and intensity of emission from the molecular chains, but they do not dictate the intrinsic coherence of the superradiant states. Our studies shed light on the optical properties of molecular collective states and their interaction with nanoscopically localized plasmons.
Abstract Interactions between a single emitter and cavity provide the archetypical system for fundamental quantum electrodynamics. Here we show that a single molecule of Atto647 aligned using DNA origami interacts coherently with a sub-wavelength plasmonic nanocavity, approaching the cooperative regime even at room temperature. Power-dependent pulsed excitation reveals Rabi oscillations, arising from the coupling of the oscillating electric field between the ground and excited states. The observed single-molecule fluorescent emission is split into two modes resulting from anti-crossing with the plasmonic mode, indicating the molecule is strongly coupled to the cavity. The second-order correlation function of the photon emission statistics is found to be pump wavelength dependent, varying from g (2) (0) = 0.4 to 1.45, highlighting the influence of vibrational relaxation on the Jaynes-Cummings ladder. Our results show that cavity quantum electrodynamic effects can be observed in molecular systems at ambient conditions, opening significant potential for device applications.
The photon blockade induced by optical nonlinearity has been widely used to generate single-photon emission under optical driving in quantum optics. However, the same approach is difficult to achieve in electrically driven molecular junctions. Here we propose a scheme for tuning photon statistics via Fano-like interference effect in a system consisting of two molecules within one optical cavity. Under electrical pumping, a transition from photon bunching to antibunching takes place as a manifestation of the Fano-like interference. This effect persists even in the presence of the dipole-dipole interaction between molecules based on the parameters extracted from the experiments. Our proposal can be realized in current-carrying scanning tunneling microscope junctions.