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arXiv:2609.00138

Collective dressed states for inelastic light scattering by atomic ensembles

Sébastien Lucas, David Wilkowski, Christian Miniatura, Sergey E. Skipetrov

physics.atom-phphysics.opticsquant-phSubmitted Aug 31, 2026• Announced Sep 2, 2026• 0 citations
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Abstract

We develop a general dressed-state framework for computing fluorescence spectra, probe absorption spectra, and photon-photon correlations of light scattered by ensembles of $N_\mathrm{at}$ two-level atoms with arbitrary $J_g \to J_e$ transitions driven by intense coherent fields. The approach employs a full vectorial treatment of the electromagnetic field, handles any atomic geometries, illumination directions, and polarizations, and yields optical observables as explicit sums of Lorentzian lines whose positions, widths, and weights are directly tied to the eigenvalues and eigenvectors of the Lindbladian. The framework is implemented in an open-source Python package and benchmarked against exact single- and two-atom calculations. We identify geometries in which the full vectorial description is essential, and the scalar approximation fails qualitatively. Applying the method to pairs of atoms with a $J_g=0\to J_e=1$ transition, we show that elastic and inelastic scattered intensities collapse onto universal master curves controlled by a single collective saturation parameter built from the dominant superradiant mode, across several orders of magnitude in drive strength and interatomic distance. We identify collective phenomena that require a description beyond this single-mode picture. Extending the analysis to atoms with ground-state degeneracy, we find that most collective features carry over, while two qualitatively new effects emerge: an incoherent spontaneous Raman channel that modifies the scaling of inelastic emission, and a slow timescale in the time-delayed correlations $g^{(2)}(τ)$ governed by the competition between Raman scattering and subradiant decay, controlled by a single dimensionless parameter. These results provide both physical insight and practical computational tools for engineering collective optical responses in few-atom systems such as optical tweezer arrays.

Comments
40 pages, 21 figures, accompanied by a Python package for reproducing the data

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Microscopic models based on multilevel atoms are central to optimizing nonlinear optical responses and the coherent control of light. These models are traditionally based on single-atom effects that are parametrically extrapolated to include collective effects, such as an enhanced response or propagation within atomic media. In this work, we present a systematic analysis of the cooperative effects arising in driven systems composed of multilevel atoms coupled via a common electromagnetic environment. The analysis is based on an interplay between dressed states induced by the driving field and photon exchanges, and collective decay channels. This theory is applied to the case of four-wave mixing induced by a pair of lasers acting on an atomic pair with internal levels in the diamond configuration. The effect of interatomic correlations and collective decay over the photons created in this nonlinear process is then explored. We identify three regions of operation: (i) laser-dominated, (ii) intermediate, and (iii) dipole-dominated. The dependence of single- and two-photon correlations is studied in detail for each region by varying atomic orientations and laser parameters consistent with current experiments involving atomic gases. Photonic correlation functions are shown to exhibit a transition from a Lorentz-like dependence on the two-photon detuning—with general features that can be obtained in an isolated atom scheme—to a two-peaked distribution when the dipole-dipole interactions become relevant. For weak Rabi frequencies whose value is smaller than the highest collective decay rate, the atoms are trapped inside their ground state as they approach each other. It is found that the anisotropy of the dipole-dipole interaction and its wave nature are essential to understand the behavior of the photon correlations. Signatures of these processes are identified for existing experimental realizations. The intuition obtained from this connection helps to uncover relevant parameters that could be exploited for quantum control protocols based on dispersive and dissipative cooperative effects in multilevel systems.
We derive equations for the strongly coupled system of light and dense atomic ensembles. The formalism includes an arbitrary internal-level structure for the atoms and is not restricted to weak excitation of atoms by light. In the low-light-intensity limit for atoms with a single electronic ground state, the full quantum field-theoretical representation of the model can be solved exactly by means of classical stochastic electrodynamics simulations for stationary atoms that represent cold atomic ensembles. Simulations for the optical response of atoms in a quantum degenerate regime require one to synthesize a stochastic ensemble of atomic positions that generates the corresponding quantum statistical position correlations between the atoms. In the case of multiple ground levels or at light intensities where saturation becomes important, the classical simulations require approximations that neglect quantum fluctuations between the levels. We show how the model is extended to incorporate corrections due to quantum fluctuations that result from virtual scattering processes. In the low-light-intensity limit, we illustrate the simulations in a system of atoms in a Mott-insulator state in a two-dimensional optical lattice, where recurrent scattering of light induces strong interatomic correlations. These correlations result in collective many-atom subradiant and superradiant states and a strong dependence of the response on the spatial confinement within the lattice sites.
We study the collective optical response of an atomic ensemble confined within a single-mode optical cavity by stochastic electrodynamics simulations that include the effects of atomic position correlations, internal level structure, and spatial variations in cavity coupling strength and atom density. In the limit of low light intensity, the simulations exactly reproduce the full quantum field-theoretical description for cold stationary atoms and at higher light intensities we introduce semiclassical approximations to atomic saturation that we compare with the exact solution in the case of two atoms. We find that collective subradiant modes of the atoms, with very narrow linewidths, can be coupled to the cavity field by spatial variation of the atomic transition frequency and resolved at low intensities, and show that they can be specifically driven by tailored transverse pumping beams. We show that the cavity optical response, in particular both the subradiant mode profile and the resonance shift of the cavity mode, can be used as a diagnostic tool for the position correlations of the atoms and hence the atomic quantum many-body phase. The quantum effects are found to be most prominent close to the narrow subradiant mode resonances at high light intensities. Although an optical cavity can generally strongly enhance quantum fluctuations via light confinement, we show that the semiclassical approximation to the stochastic electrodynamics model provides at least a qualitative agreement with the exact optical response outside the subradiant mode resonances even in the presence of significant saturation of the atoms.
The interaction between light and matter has captivated physicists for centuries, from early studies of vision and refraction in ancient Greece to the development of quantum mechanics and quantum electrodynamics in the past century. While the response of a single quantum emitter to light is well understood, the radiative properties of an ensemble of closely spaced emitters are far more intricate. Coupling to a shared electromagnetic environment induces coherent and dissipative interactions between emitters, giving rise to a collective response that cannot be captured by treating them independently. In the regime of few excitations, the system hosts delocalized subradiant states, that is, coherent superpositions that are largely decoupled from the electromagnetic field and thus decay at suppressed rates. While this weak coupling makes subradiant states attractive for quantum technologies, it also renders them difficult to manipulate. At higher excitation densities, the intrinsic nonlinearity of emitters and the exponential growth of the Hilbert space make theoretical and numerical descriptions of the system and its dynamics increasingly challenging. This thesis explores two fundamental questions: How can subradiant and dark states be selectively accessed and harnessed for practical applications in quantum technologies? And how can interacting ensembles of quantum emitters be efficiently simulated to uncover their many-body physics? The first part of the thesis develops protocols for controlling and addressing dark states in free-space and waveguide-coupled atomic arrays, demonstrating their utility in quantum storage and the deterministic generation of entangled photonic states. Incorporating atomic motion, we further show that collective subradiant states can enhance cooling in dense atomic arrays, offering new avenues for controlling motional dynamics. In the second part, we introduce cumulant expansions of the equations of motion as a powerful tool to analytically and numerically investigate collective decay in the many-body regime. We first examine the collective decay of fully excited atomic arrays in free space, characterizing the onset and scaling of the superradiant burst across different geometries. In collaboration with experiments on ultracold erbium atoms in optical lattices, we provide the first direct observations of many-body collective effects in free-space ordered arrays, including early-time superradiant bursts, late-time subradiant tails, and the emergence of atomic correlations throughout the dynamics. Finally, we theoretically and numerically explore the transient formation of multi-excitation subradiant states, and demonstrate how the existence of multiple dissipation channels suppresses steady-state superradiance in extended arrays.
Collective coupling between dipoles can dramatically modify the optical response of a medium. Such effects depend strongly on the geometry of the medium and the polarization of the light. Using a classical coupled dipole model, here we investigate the simplest case of one-dimensional arrays of interacting atomic dipoles driven by a weak laser field. Changing the polarization and direction of the driving field allows us to separately address superradiant, subradiant, redshifted, and blueshifted eigenmodes, as well as observe strong Fano-like interferences between different modes. The cooperative eigenvectors can be characterized by the phase difference between nearest-neighbor dipoles, ranging from all oscillating in phase to all oscillating out of phase with their nearest neighbors. Investigating the eigenvalue behavior as a function of atom number and lattice spacing, we find that certain eigenmodes of an infinite atomic chain have the same decay rate as a single atom between two mirrors. The effects we observe provide a framework for collective control of the optical response of a medium, giving insight into the behavior of more complicated geometries, as well as providing further evidence for the dipolar analog of cavity QED.
An ensemble of atoms coupled to the radiation field exhibits collective behaviours when the interatomic separation is comparable to the wavelength of photons emitted by the atoms. The collective coupling of the atoms with the electromagnetic field gives rise to coherent exchange interactions between the atoms. In addition, the spontaneous decay of photons from the ensemble becomes a collective process that can happen at a much faster (superradiant) or slower (subradiant) rate than that of a single atom. These processes affect the way that fluorescence light is scattered from the system when it is driven by a laser. However, little is known about the response of a dense atomic gas beyond the linear regime of very weak driving, due to the involved complexity of the problem. The first part of this thesis investigates how the presence of strong laser driving affects properties of the far-field fluorescence light emitted by the ensemble, such as the power spectrum and second order coherence. Depending on the strength of the driving laser and the particular arrangement of the atoms, the laser can modify considerably how the collective behaviours of the atomic ensemble are manifested in the fluorescence. The relative strengths of the coherent interaction and collective decay process are intrinsically linked to the way that the atoms couple to the radiation field; one cannot be changed without modifying the other. Altering the environment by, for example, placing the atoms near a surface or a waveguide, can change this relation significantly from that for atoms in free space. Therefore, modified environments represent a platform for the generation of otherwise inaccessible regimes of collective behaviour, with potential applications in quantum state engineering. The second part of this thesis provides a numerical investigation into how the collective properties of a dense atomic system can be manipulated by placing the atoms close to planar surfaces or an optical nanofiber. These structures modify the light-matter coupling by altering the electric field experienced by the atoms. It is shown that surfaces of metallic and dielectric materials can be used to either enhance or suppress the collective behaviours, depending on the particular system arrangement. In particular, the coupling of atoms with bound surface modes, such as the surface plasmon polaritons that are formed at an air-metal interface, is demonstrated to have a strong effect on the interactions. An optical nanofiber supports a set of fundamental guided modes, that propagate along the fiber. If the atoms are suitably polarised, then they will emit primarily into the guided modes travelling in one direction. By calculating and analysing the collective decay states of a chain of atoms placed near a nanofiber, it is demonstrated that the atom-fiber coupling leads to the formation of a superradiant mode that is preserved at large atomic separations. The presence of chiral emission is shown to introduce phase gradients to the collective modes.