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arXiv:2512.05196

Multimode equilibrium approximations in light-matter systems from weak to strong coupling

Davis M. Welakuh, Vasil Rokaj, Michael Ruggenthaler, Angel Rubio

quant-phSubmitted Dec 4, 2025• Announced Dec 8, 2025• 0 citations
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Abstract

In this work, we detail different approaches to treat multi-mode photonic environments within non-relativistic quantum electrodynamics in the long-wavelength approximation efficiently. Specifically we show that for equilibrium properties of coupled light-matter systems, we can approximately capture the effects of multi-mode photonic environments on matter systems by either only keeping the polarization part of the electric field in the length-gauge formulation or by a few effective modes. We present a comprehensive set of approximation methods designed to accurately capture equilibrium phenomena in quantum light-matter systems across a range of complex photonic environments, from weak to strong coupling. These methods are applied to atomic and molecular models as well as to a two-dimensional quantum ring, demonstrating the versatility of our approach and laying the groundwork for first-principles simulations of real materials in cavity quantum electrodynamics.

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17 pages, 9 figures

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In this work, we detail different approaches to treat multi-mode photonic environments within non-relativistic quantum electrodynamics in the long-wavelength approximation efficiently. Specifically we show that for equilibrium properties of coupled light-matter systems, we can approximately capture the effects of multi-mode photonic environments on matter systems by either only keeping the polarization part of the electric field in the length-gauge formulation or by a few effective modes. We present a comprehensive set of approximation methods designed to accurately capture equilibrium phenomena in quantum light-matter systems across a range of complex photonic environments, from weak to strong coupling. These methods are applied to atomic and molecular models as well as to a two-dimensional quantum ring, demonstrating the versatility of our approach and laying the groundwork for first-principles simulations of real materials in cavity quantum electrodynamics.
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Room-temperature cavity quantum electrodynamics with molecular materials in optical cavities offers exciting prospects for controlling electronic, nuclear and photonic degrees of freedom for applications in physics, chemistry and materials science. However, achieving strong coupling with molecular ensembles typically requires high molecular densities and substantial electromagnetic-field confinement. These conditions usually involve a significant degree of molecular disorder and a highly structured photonic density of states. It remains unclear to what extent these additional complexities modify the usual physical picture of strong coupling developed for atoms and inorganic semiconductors. Using a microscopic quantum description of molecular ensembles in realistic multimode optical resonators, we show that the emergence of vacuum Rabi splitting in linear spectroscopy is a necessary but not sufficient metric of coherent admixing between light and matter. In low-finesse multi-mode situations, we find that molecular dipoles can be partially hybridized with photonic dissipation channels associated with off-resonant cavity modes. These vacuum-induced dissipative processes ultimately limit the extent of light-matter coherence that the system can sustain.This article is part of the theme issue 'The quantum theory of light'.
Recent technological developments have made it increasingly easy to access the non-perturbative regimes of cavity quantum electrodynamics known as ultrastrong or deep strong coupling, where the light-matter coupling becomes comparable to the bare modal frequencies. In this work, we address the adequacy of the broadly used single-mode cavity approximation to describe such regimes. We demonstrate that, in the non-perturbative light-matter coupling regimes, the single-mode models become unphysical, allowing for superluminal signalling. Moreover, considering the specific example of the quantum Rabi model, we show that the multi-mode description of the electromagnetic field, necessary to account for light propagation at finite speed, yields physical observables that differ radically from their single-mode counterparts already for moderate values of the coupling. Our multi-mode analysis also reveals phenomena of fundamental interest on the dynamics of the intracavity electric field, where a free photonic wavefront and a bound state of virtual photons are shown to coexist.
Abstract Recent technological developments have made it increasingly easy to access the non-perturbative regimes of cavity quantum electrodynamics known as ultrastrong or deep strong coupling, where the light–matter coupling becomes comparable to the bare modal frequencies. In this work, we address the adequacy of the broadly used single-mode cavity approximation to describe such regimes. We demonstrate that, in the non-perturbative light–matter coupling regimes, the single-mode models become unphysical, allowing for superluminal signalling. Moreover, considering the specific example of the quantum Rabi model, we show that the multi-mode description of the electromagnetic field, necessary to account for light propagation at finite speed, yields physical observables that differ radically from their single-mode counterparts already for moderate values of the coupling. Our multi-mode analysis also reveals phenomena of fundamental interest on the dynamics of the intracavity electric field, where a free photonic wavefront and a bound state of virtual photons are shown to coexist.
Strong light-matter coupling enables hybrid states in which photonic and electronic degrees of freedom become correlated even in the ground state. While many-body effects in long-range dispersion interactions are known to reshape electronic properties under such conditions, their impact on quantum-optical observables remains largely unexplored. Here, we address this problem using quantum electrodynamical density-functional theory (QEDFT) combined with the recently developed photon-many-body dispersion (pMBD) functional, which can capture higher-order electron-photon correlations and multi-photon processes. We compute ground-state photonic observables including photon number fluctuations, second-order correlations, and quadrature variances, and find squeezing and super-Poissonian photon statistics emerging from light-matter interactions in the strong coupling regime. Our results demonstrate that capturing the full hierarchy of many-body, electron-photon and multi-photon correlations is essential for a consistent description of quantum-optical properties in strongly coupled molecular systems, establishing QEDFT as a first-principles framework for predicting nonclassical photonic features in the ground state of complex systems.
Room temperature cavity quantum electrodynamics with molecular materials in optical cavities offers exciting prospects for controlling electronic, nuclear and photonic degrees of freedom for applications in physics, chemistry and materials science. However, achieving strong coupling with molecular ensembles typically requires high molecular densities and substantial electromagnetic field confinement. These conditions usually involve a significant degree of molecular disorder and a highly structured photonic density of states. It remains unclear to what extent these additional complexities modify the usual physical picture of strong coupling developed for atoms and inorganic semiconductors. Using a microscopic quantum description of molecular ensembles in realistic multimode optical resonators, we show the that the emergence of a vacuum Rabi splitting in linear spectroscopy is a necessary but not sufficient metric of coherent admixing between light and matter. In low finesse multi-mode situations we find that molecular dipoles can be partially hybridised with photonic dissipation channels associated with off-resonant cavity modes. These vacuum-induced dissipative processes ultimately limit the extent of light-matter coherence that the system can sustain.