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arXiv:2509.03067 · Nanophotonics

Theory of dynamical superradiance in organic materials

Lukas Freter, Piper Fowler-Wright, Javier Cuerda, Brendon W. Lovett, Jonathan Keeling, Päivi Törmä

Published Dec 1, 2025• 1 citation
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Abstract

We develop the theory of dynamical superradiance - the collective exchange of energy between an ensemble of initially excited emitters and a single-mode cavity - for organic materials where electronic states are coupled to vibrational modes. We consider two models to capture the vibrational effects: first, vibrations treated as a Markovian bath for two-level emitters, via a pure dephasing term in the Lindblad master equation for the system; second, vibrational modes directly included in the system via the Holstein-Tavis-Cummings Hamiltonian. By exploiting the permutation symmetry of the emitters and weak U(1) symmetry, we develop a numerical method capable of exactly solving the Tavis-Cummings model with local dissipation for up to 140 emitters. Using the exact method, we validate mean-field and second-order cumulant approximations and use them to describe macroscopic numbers of emitters. We analyze the dynamics of the average cavity photon number, electronic coherence, and Bloch vector length and show that the effect of vibrational mode coupling goes beyond simple dephasing. Our results show that superradiance is possible in the presence of vibrational mode coupling; for negative cavity detunings, the vibrational coupling may even enhance superradiance. We identify asymmetry of the photon number rise time as a function of the detuning of the cavity frequency as an experimentally accessible signature of such vibrationally assisted superradiance.

DOI
10.1515/nanoph-2025-0427

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We develop the theory of dynamical superradiance - the collective exchange of energy between an ensemble of initially excited emitters and a single-mode cavity - for organic materials where electronic states are coupled to vibrational modes. We consider two models to capture the vibrational effects: first, vibrations treated as a Markovian bath for two-level emitters, via a pure dephasing term in the Lindblad master equation for the system; second, vibrational modes directly included in the system via the Holstein-Tavis-Cummings Hamiltonian. By exploiting the permutation symmetry of the emitters and weak U(1) symmetry, we develop a numerical method capable of exactly solving the Tavis-Cummings model with local dissipation for up to 140 emitters. Using the exact method, we validate mean-field and second-order cumulant approximations and use them to describe macroscopic numbers of emitters. We analyze the dynamics of the average cavity photon number, electronic coherence, and Bloch vector length and show that the effect of vibrational mode coupling goes beyond simple dephasing. Our results show that superradiance is possible in the presence of vibrational mode coupling; for negative cavity detunings, the vibrational coupling may even enhance superradiance. We identify asymmetry of the photon number rise time as a function of the detuning of the cavity frequency as an experimentally accessible signature of such vibrationally assisted superradiance.
The Tavis–Cummings system, wherein emitters collectively interact with the same optical mode, has been a long-standing model to study collective photon emission phenomena such as superradiance. However, disorder in the resonant frequencies of the quantum emitters can perturb these effects. In this paper, we study the impact of dynamic modulation on the interplay between superradiance and spectral disorder. Through numerical simulations and analytical calculations, we provide evidence that the effective cooperativity of the superradiant mode can be multiplicatively enhanced with a quantum control protocol modulating the resonant frequency of the optical mode. Our results are relevant to experimental demonstration of superradiance in solid-state quantum optical systems, wherein the spectral disorder is a signficant technological impediment toward achieving photon-mediated emitter–emitter couplings.
In this study, we present the superradiance effects of N identical molecular emitters inside Fabry–Pérot (FP) cavity systems in the framework of macroscopic quantum electrodynamics. The proposed theory can estimate the enhancement of spontaneous emission rates, including the effects of cavity geometry and material dielectric properties. Moreover, our study connects the multichromophoric excitation energy transfer theory and the Tavis–Cummings model via identical cooperative decay rates and dipole–dipole shifts. For molecules resonant with the cavity photon mode, we find that the enhancement is not exactly proportional to N even in a perfect FP cavity due to the effects of electrostatic dipole–dipole interactions. Moreover, in a silver FP cavity, our simulation shows that the enhancement saturates for a large N, indicating that the cavity photon mode can lead to only the collective emission of a limited number of molecules. For molecules in the proximity of the silver mirror, we demonstrate that under specific conditions, the subradiance of molecular emitters can occur through surface plasmon polaritons. Our study not only provides new insights into the mechanism of superradiance effects but also demonstrates that collective effects such as superradiance and subradiance can be controlled by manipulating the dielectric environments.
We investigate the emergence of cooperative radiation phenomena in ensembles of two-level atoms coupled to a lossy resonant cavity beyond the Markovian and mean-field approximations. By deriving a complete analytical solution for the two-emitter case and employing a numerically exact method for larger ensembles, we characterize the full transition from Markovian to non-Markovian collective dynamics for systems of up to 10310^3103 emitters. Our results reveal three distinct regimes: a Markovian phase exhibiting the standard superradiant burst, a non-Markovian phase featuring spontaneous superabsorption of the emitted field, and a critical regime marked by pulsed collective emission. We show that the critical spectral width separating these behaviors increases monotonically with the number of emitters, demonstrating that environmental memory effects can be enhanced by cooperativity. Finally, we find that the superradiant scaling of the peak intensity progressively degrades with increasing system size, approaching a subquadratic law in the limit of a perfect cavity. In this regime, spontaneous superabsorption emerges as a distinct manifestation of non-Markovian cooperativity.
The interaction of an ensemble of NNN two-level quantum emitters with a single-mode electromagnetic field is described by the Tavis-Cummings model. There, the collectively enhanced light-matter coupling strength is given by gN=Ng‾1{g}_{N}=\sqrt{N}{\overline{g}}_{1}gN​=N​g​1​, where g‾1{\overline{g}}_{1}g​1​ is the ensemble-averaged single-emitter coupling strength. This model has been employed to describe and to analyze numerous cavity-based experiments. Here, we show that this is only justified if the effective scattering rate into noncavity modes is negligible compared to the cavity's free-spectral range. In terms of experimental parameters, this requires that the optical depth of the ensemble is low, a condition that is violated in several state-of-the-art experiments. We give quantitative conditions for the validity of the Tavis-Cummings model and derive a more general Hamiltonian description that takes into account the cascaded interaction of the photons with all consecutive emitters. We show that the predictions of our cascaded model can differ quantitatively and even qualitatively from those obtained with the Tavis-Cummings model. Finally, we present experimental data, for which the deviation from the predictions of the Tavis-Cummings model is apparent. Our findings are relevant for all experiments in which optically dense ensembles of quantum emitters are coupled to an optical resonator.
Collective radiance effects in quantum degenerate systems, such as superradiance and subradiance of a partially inverted ensemble, are shaped by the interplay of spatial confinement and exchange statistics. We investigate this interplay using a purely dissipative field theoretic quartic Lindblad master equation, which captures the nonlinear dynamics of the combined motional and electronic manifolds. This approach captures the interplay between the permutational symmetry of the Lindbladian and the exchange symmetry of the particles, quantifying how bosonic enhancement and Pauli blocking dictate superradiant and subradiant scaling. We identify two distinct routes to distinguishable dynamics: thermal dilution of the initial state at high temperatures and the dynamical breakdown of collective order via recoil induced transport in soft traps. This analysis provides a benchmark for collective emission in quantum-degenerate atomic systems with coupled motional and internal dynamics, such as optical lattice clocks and spinor gases, when dissipation is engineered to control recoil and motional heating.
Abstract We consider the superradiant transition of a generalized Tavis–Cummings model, where a number of two-level qubits are coupled to a dissipative cavity. The cavity is coherently driven through a parametric medium, and all-to-all interactions between the qubits are introduced. While the nonlinear gain from the parametric drive breaks the U (1) symmetry of the standard Tavis–Cummings model, thus giving rise to superradiance with squeezed cavity fields, we show that the interactions impact the collective excitations and significantly modify the superradiant transition. Insights into the superradiant phase transitions, as well as the interaction effects, are obtained through effective models involving only a handful of low-lying collective states, under which the steady-state phase diagram of the hybrid system is faithfully reproduced. Our study is relevant to Rydberg-atom arrays coupled to a parametrically driven cavity, where the long-range interactions derive from the dipole–dipole interatomic interactions.