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arXiv:2601.11297

Microscopic quantum description of surface plasmon polaritons: Revealing intrinsic ultrastrong light-matter coupling

Florian Maurer, Thomas F. Allard, Yanko Todorov, Guillaume Weick, David Hagenmüller

physics.opticscond-mat.mes-hallquant-phSubmitted Jan 16, 2026• Announced Jan 19, 2026• Revised Jul 27, 2026 (v2)
v1 · Jan 16, 2026v2 · Jul 27, 2026
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Abstract

We develop a microscopic quantum theory of surface plasmon polaritons valid for arbitrary metal-dielectric geometries. Our framework is based on the Power-Zienau-Woolley representation of quantum electrodynamics, which provides an optimal separation between electronic and photonic degrees of freedom and is therefore particularly well suited for constructing quantum descriptions of polaritonic excitations in strongly dispersive media. Within this formulation, the fundamental electronic oscillator is identified as the bulk plasmon mode, which is nonperturbatively coupled to the radiative continuum of free photon modes. This coupling induces a geometry-dependent renormalization of the bulk plasma frequency, giving rise to confined plasmonic resonances. As specific applications, we recover the localized surface plasmon modes of metallic nanoparticles, including radiative frequency shifts and decay, as well as the exact dispersion relation of propagating surface plasmon polaritons at planar interfaces. Our quantum treatment further reveals that light-matter interactions at metal-dielectric interfaces are inherently in the ultrastrong coupling regime. As a result, in the quasistatic limit, the system exhibits unconventional ground-state quantum fluctuations that can be controlled through the refractive index. These results open new intriguing perspectives in the field of quantum plasmonics.

Journal reference
Phys. Rev. B 114, 055421 (2026)
DOI
10.1103/2pdp-zwgl
Comments
19 pages, 9 figures

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We develop a microscopic quantum theory of surface plasmon polaritons valid for arbitrary metal-dielectric geometries. Our framework is based on the Power-Zienau-Woolley representation of quantum electrodynamics, which provides an optimal separation between electronic and photonic degrees of freedom and is therefore particularly well suited for constructing quantum descriptions of polaritonic excitations in strongly dispersive media. Within this formulation, the fundamental electronic oscillator is identified as the bulk plasmon mode, which is nonperturbatively coupled to the radiative continuum of free photon modes. This coupling induces a geometry-dependent renormalization of the bulk plasma frequency, giving rise to confined plasmonic resonances. As specific applications, we recover the localized surface plasmon modes of metallic nanoparticles, including radiative frequency shifts and decay, as well as the exact dispersion relation of propagating surface plasmon polaritons at planar interfaces. Our quantum treatment further reveals that light-matter interactions at metal-dielectric interfaces are inherently in the ultrastrong coupling regime. As a result, in the quasistatic limit, the system exhibits unconventional ground-state quantum fluctuations that can be controlled through the refractive index. These results open new intriguing perspectives in the field of quantum plasmonics.
Surface plasmon polaritons are charge density waves of electrons in a metal, which are coupled to an electromagnetic field at a metal-dielectric interface. The electro- magnetic field associated with surface plasmons is confined, resulting in increased field intensities near the interface. Optical emitters placed near a metal film interact strongly with the surface plasmon modes present, not only modifying the radiation rates, but also the radiation profile. These emitters may be used to store and process information, and understanding their behaviour in the presence of a lossy metal film is important in determining the advantages and limitations of using surface plasmons. In this thesis, we wish to understand how we can optically control atoms by exploring two physical phenomena: first, the influence of surface plasmons on collective effects in an ensemble of emitters. Secondly, the single photon excitation of an emitter near a metal film. In the first case, we analyze the collective radiative behaviour of multiple classical emitters near a metal film that radiatively couple to the far-field through surface plasmon modes. We demonstrate that the contributions of dipolar image charges within the metal film significantly affect the cooperative emission of nearby sources, generating sub- and super-radiant emission that can be controlled with a suitably detuned external driving field. In the second case, we determine the excitation probability of an atom near a metal film by a single photon pulse that is time reversed. Using a quantum electro- dynamic description of absorbing dielectrics, we show that non-radiative decay will limit the excitation probability to about half of the maximum that could be achieved in the absence of losses.
Enabling the confinement of light to a scale far below the one of conventional optics, surface plasmon polaritons (SPPs) induced by an electromagnetic field in a metal-dielectric interface supply an ideal system to explore strong quantized light-matter coupling. The fast matter-SPP population exchange reported in previous works makes it a candidate for spin manipulation, but such reversible dynamics asymptotically vanishes accompanying the quantum matter relaxing completely to its ground state. Here, we study the exact dissipative dynamics of a quantum emitter (QE) coupled to SPPs. It is interesting to find that, qualitatively different from conventional findings, the QE can be partially stabilized in its excited state even in the presence of the lossy metal. Our analysis reveals that it is the formation of a QE-SPP bound state which results in such suppressed dissipation. Enriching the decoherence dynamics of the QE in the lossy medium, our result is helpful to understand QE-SPP interactions and apply plasmonic nanostructures in quantum devices.
This thesis encompasses fundamental theoretical research on plasmonics, electromagnetic coherence, and quantum complementarity.Three main topics are covered: surface-plasmon polaritons (SPPs), partial coherence of optical surface fields, and complementarity in vectorial photon interference.Existence of new SPP modes at planar single-interface and thinfilm geometries are predicted.It is further shown, for the first time, how a higher-order metal-slab mode, commonly not regarded useful, may turn into a strongly confined long-range surface mode in many situations where the fundamental long-range SPP does not exist and the single-interface SPP propagation is negligible.Partially coherent SPP fields are studied and a scheme to tailor the vectorial coherence of polychromatic SPPs in the Kretschmann setup by controlling the correlations of the source light is advanced.Generation and coherence of purely evanescent light fields are also examined.It is demonstrated that, for such fields, the coherence length in air can be notably shorter than the free-space wavelength.The analysis also reveals the possibility to excite an evanescent field that shares the polarization properties of blackbody radiation, yet with tunable coherence qualities.Polarization modulation in double-pinhole photon interference is explored to derive two general complementarity relations among distinguishability and visibility associated with genuine vector-light quantum fields of arbitrary state.The established framework uncovers a new intrinsic aspect of wave-particle duality of the photon, having no correspondence within the scalar quantum treatment.
Light-matter interactions underlie many quantum technologies, yet whether quasiparticles formed from such interactions preserve the full quantum state of light remains unresolved. Surface plasmon polaritons (SPPs), a class of polaritons formed by interacting photons with free-electron oscillations at metal-dielectric interfaces, are prime candidates to explore this question. Here we demonstrate quantum interference between single photons and SPPs using an Au-SiNx_{\mathrm{x}}x​ integrated photonic-plasmonic device. Our results reveal that SPPs retain the indistinguishability of their excitation photons, establishing SPP as a viable quantum information carrier and opening a potential route toward photonic-plasmonic quantum circuitry.
Attempting to implement quantum information related applications utilizing atoms and photons, as they naturally form quantum systems supporting superposition states, hybrid quantum plasmonic systems emerged in the past as a platform to study and engineer light-matter interaction. This platform combines the unrivaled electromagnetic field localization of surface plasmon polaritons, boosting the light-matter coupling rate, with the tremendous integration potential of truly nanoscale structures, and both the significant emission rates of nanoantennas and photonic transmission velocities. In this work, a classical description of surface plasmon polaritons is combined with a light-matter interaction model based on a cavity quantum electrodynamical formalism. The resulting composite semi-classical method, introduced and described in this thesis, provides efficient and versatile means to simulate the dynamical behavior of radiative atomic transitions coupled to plasmonic cavity modes in the weak incoherent coupling regime. Both the emission into the far field and various dissipation mechanisms are included by expanding the model to an open quantum system. The variety of light-matter interaction applications that can be modeled with the outlined method is indicated by the four different exemplary scenarios detailed in the application chapter of this thesis. The classical description of localized surface plasmon polaritons is benchmarked by reproducing the experimental measurements of the molecular fluorescence manipulation through optical nanoantennas in a collaborative effort with experimental partners. Furthermore, in the weak light-matter coupling regime, the potential of achieving a higher nanoantenna functionality and simultaneously realizing more elaborate quantum dynamics is revealed by the three remaining applications. Each pivotally involving a bimodal nanoantenna and demonstrating different quantum optical phenomena, the implementation of cavity radiation mode conversion, non-classical cavity emission statistics, and non-classical cavity emission properties is shown and described in the application chapter.
Tunable surface plasmons on the interface of a multilevel atomic medium with a cross coupling of the electric and magnetic components of a plasmonic field are investigated. The strong chirality resulting from the quantum coherence leads to some exciting properties of the surface plasmons. Compared to the traditional chiral-metal interface, surface plasmonic mode can still be found at the interface between such atomic media and a dielectric even when both the permittivity and the permeability of the medium are positive. This is in contrast to the conventional plasmonic systems where the signs of the permittivities or permeabilities on the two sides of the interface are opposite. We call this phenomenon an electromagnetically induced plasmon. Additionally, as the chirality and effective refractive index of the atomic medium are dependent on the intensity and phase of the controlling field, we can conveniently manipulate the properties of the surface plasmons.