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arXiv:2608.19336

Multipolar Light-Matter Hamiltonians in Symmetry-Breaking Photonic Vacuums

Liu Yang, Jiadu Lin, Qing-Dong Jiang

quant-phcond-mat.otherphysics.atom-phphysics.opticsSubmitted Aug 19, 2026• Announced Aug 21, 2026• 0 citations
arXivHTMLPDF

Abstract

We show that the conventional multipolar Hamiltonian is qualitatively modified when the photonic vacuum breaks inversion or time-reversal symmetry. By explicitly applying the Power-Zienau-Woolley transformation, we derive the resulting multipolar Hamiltonians for two idealized chiral photonic environments: a spatial-chiral vacuum, which breaks inversion symmetry, and a temporal-chiral vacuum, which breaks time-reversal symmetry. In the spatial-chiral case, the transformation generates an inversion-breaking self-energy, whereas in the temporal-chiral case it produces an additional Zeeman-like energy. Using a trapped hydrogen-like atom and a charged harmonic oscillator in cavities as minimal examples, we show that these symmetry-dependent terms lead to characteristic spectral shifts. Our work provides a general framework for describing light-matter interactions in chiral quantum electrodynamics and identifying the associated symmetry-dependent effects on cavity-embedded atoms, molecules, and quantum materials.

Comments
7 pages, 3 figures, 1 table; Supplemental Material available as an ancillary file

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We show that the conventional multipolar Hamiltonian is qualitatively modified when the photonic vacuum breaks inversion or time-reversal symmetry. By explicitly applying the Power-Zienau-Woolley transformation, we derive the resulting multipolar Hamiltonians for two idealized chiral photonic environments: a spatial-chiral vacuum, which breaks inversion symmetry, and a temporal-chiral vacuum, which breaks time-reversal symmetry. In the spatial-chiral case, the transformation generates an inversion-breaking self-energy, whereas in the temporal-chiral case it produces an additional Zeeman-like energy. Using a trapped hydrogen-like atom and a charged harmonic oscillator in cavities as minimal examples, we show that these symmetry-dependent terms lead to characteristic spectral shifts. Our work provides a general framework for describing light-matter interactions in chiral quantum electrodynamics and identifying the associated symmetry-dependent effects on cavity-embedded atoms, molecules, and quantum materials.
Based on a hybrid light-matter unitary transformation for cavity quantum electrodynamics, we investigate the spectral shift of an atom induced by quantum fluctuations in a chiral vacuum cavity. Remarkably, we find an intriguing angular momentum dependent shift in the spectra of bound states. Our approach shows promise in going beyond traditional perturbative methods and demonstrates effectiveness even in the strong-coupling limit, as evidenced by our numerical benchmarks in the case of a two-dimensional quantum harmonic oscillator. In addition, we establish a cavity-interaction picture for calculating the chiral vacuum Rabi oscillation in the strong-coupling limit for a generic central potential. The anomalous spectral shift revealed in this study possesses both fundamental and practical significance and could be readily observed in experiments.
Structured light offers a powerful approach to tailor light--matter interactions in quantum systems with chiral properties. While chirality has been extensively studied in passive platforms, the role of optical gain in controlling chiral quantum dynamics remains largely unexplored. In this work, we develop a general theoretical framework to describe the dynamics of an atomic system interacting with structured gain environments, where amplification depends on the light's polarization or momentum. By quantizing the electromagnetic field in linear bianisotropic media with gain and extending the Lindblad formalism to these settings, we derive a master equation governing the atom's irreversible evolution. We show that chiral gain can break time-reversal symmetry and drive the system toward a symmetry-broken steady state with nonreciprocal properties. This effect is illustrated in detail for moving plasmonic substrates, which exhibit inherently chiral gain that selectively amplifies transitions of a given handedness. Our results establish chiral gain as a novel mechanism for engineering nonreciprocal quantum steady states.
Multipolar quantum optics deals with the interaction of light with matter as a many-body bound system of charged particles where the coupling to electromagnetic fields is in terms of the multipolar electric polarization and magnetization. We describe two transformations applied to the conventional non-relativistic formalism, namely a gauge transformation applied directly to the fields at the Lagrangian stage and a unitary transformation applied to the old Hamiltonian. We show how such transformations lead to the same Power-Zienau-Woolley (PZW) formulation of the quantum electrodynamics (QED) of an overall electrically neutral many-body bound system of charges, including the internal motion as well as the gross dynamics of the centre of mass. Besides highlighting the utility of the multipolar formalism as a reliable and convenient platform in dealing with optical processes in atomic and molecular physics, it is shown how the analysis can also lead to the identification of the Röntgen effect arising from the gross motion of an electric dipole moment in a magnetic field and the Aharonov-Casher effect due to the motion of a magnetic dipole moment in an electric field. The importance of the two effects is pointed out in both experimental and theoretical contexts.This article is part of the theme issue 'The quantum theory of light'.
We reveal that a chiral cavity distinguishes the resonant and antiresonant interactions between a two-dimensional electron gas and the cavity vacuum. For co-rotating helicities, the modes anticross, exhibiting vacuum Rabi splitting, and retain a bare vacuum ground state. For counter-rotating helicities, the modes cross, acquiring vacuum-mediated energy shifts and a two-mode squeezed ground state. We trace the origin of these observations to the SU(2) and SU(1,1) symmetries of the respective Hamiltonians and present their spectroscopic signatures in chiral photonic crystal cavities. We further predict that cavity chirality produces a handedness-dependent correction to Hall resistivity at finite polariton broadening, while such a correction is not present in an achiral cavity. For the longitudinal resistivity, we find an asymmetric response of the Shubnikov--de Haas oscillations for the different helicities. Finally, we present an experimentally accessible route for detecting the squeezed ground state through current fluctuations. Parameters based on a recently demonstrated terahertz chiral cavity place these effects within experimental reach.
We present a general theoretical framework to capture light-matter interactions beyond the electric-dipole approximation (EDA), applicable to extended nano- and microscale materials interacting with spatially structured electric fields without truncation at finite multipolar order. The approach is based on the Power-Zienau-Woolley (PZW) Hamiltonian for light-matter interactions and a representation of the material's Hamiltonian in a basis of maximally localized Wannier functions (MLWFs), obtainable from first-principles calculations. We utilize this approach to clarify the limitations of the ubiquitous dipole approximation. We consider electric fields with both uniform and non-uniform intensities and a range of ratios of system size to the wavelength of light. Through this analysis, we identify the conditions under which the EDA breaks down, leading to significant errors in the light-induced dynamics. Contrary to conventional belief, we find that the EDA is remarkably robust for uniformly illuminated 1-D or 2-D materials when light propagates perpendicular to the material. For 3-D materials or non-perpendicular illumination of lower-dimensional materials, conventional wisdom holds and the EDA begins to break down when the wavelength becomes comparable to the system size. Furthermore, the EDA fails when the material is illuminated partially or non-uniformly. For slowly varying field intensities this failure can be corrected by finite-order multipolar corrections. However, for fields that vary substantially, correcting via multipolar terms becomes computationally impractical. In contrast, our approach captures beyond-dipole light-matter interactions at the computational cost of a standard dipole calculation. This efficiency enables accurate first-principles simulations of spatially structured light-matter dynamics in nanoscale devices, quantum materials, and interfaces.
In this study, we explore the breaking of time-reversal symmetry in a scalable cavity quantum electrodynamics (QED) lattice. Such a lattice consists of triangular cells of three cavities coupled to a two-level atom. We synthesize artificial magnetic fields to enable the chiral transfer of photons by sinusoidally modulating the cavity frequencies. Considering various configurations with different numbers of cells in the system, we analyze the circulation of photons and investigate the effect of the frequency modulation on the control of the state transfer in the system. We show the breaking and sustaining of time-reversal symmetry in certain system geometries and consider the scalability of the generating synthetic magnetic field in the system. Our study highlights the potential of scalable cavity QED lattices with synthetic magnetic fields as a versatile tool for investigating quantum phenomena and shows the utility of these systems to serve as test beds for the simulation of condensed matter systems in quantum optical settings.