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arXiv:2108.08397 · ACS Photonics

Enhancing Superradiance in Spectrally Inhomogeneous Cavity QED Systems with Dynamic Modulation

Alexander D. White, Rahul Trivedi, Kalyan Narayanan, Jelena Vuckovic A

Published Jun 16, 2022• 8 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1021/acsphotonics.2c00581

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•Jul 7, 2021•1 citation
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.
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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.
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.
The realization and control of collective quantum effects so far have predominantly focused on cold atomic ensembles. Quantum photonic platforms, with their engineered Green's functions and integration capability of advanced solid-state quantum emitters, provide opportunities to explore regimes of light-matter interaction beyond the scope of atomic systems. In this work, we demonstrate that embedding quantum emitters within a thin dielectric layer fundamentally alters their collective radiative behavior. The optical modes in the dielectric layer mediate long-range dipole-dipole interactions between emitters, enabling both total and directional superradiance between emitters separated by several wavelengths. Crucially, this mechanism supports Dicke superradiance even in parameter regimes where standard settings fail to support an interaction, unveiling a dimensionality-driven enhancement of cooperative effects. By bridging many-body quantum optics and photonic engineering, our work reveals a distinct interplay between surrounding dimensionality and collective quantum dynamics. Experimental realization of these predictions, readily achievable in solid-state quantum optics platforms, paves the way for scalable, directional quantum light sources and frontiers in many-body quantum optics.
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.
Quantum cooperativity is evident in light-matter platforms where quantum emitter ensembles are interfaced with confined optical modes and are coupled via the ubiquitous electromagnetic quantum vacuum. Cooperative aspects such as dipole-dipole interactions and subradiance find applications in the design of nanoscale coherent light sources and highly-reflective quantum metasurfaces made up of hundreds of optically trapped atoms, in the implementation of topological quantum optics on subwavelength arrays of emitters, in quantum metrology and quantum information. The quick bursts of radiation from a collection of quasi-indistiguishable emitters provides an alternative approach to standard lasers by introducing superradiant lasers operating at extremely low intracavity power. This tutorial provides a set of theoretical tools to tackle the behavior responsible for the onset of cooperativity in light-matter systems by extending open quantum system dynamics methods, such as the master equation and quantum Langevin equations, to electron-photon interactions in strongly coupled and correlated quantum emitters ensembles. These analytical approaches are then also extended to frequency disordered or vibronically coupled quantum emitter ensembles with wide relevance ranging from atoms in optical lattices, quantum dots in solid state environments or molecular quantum systems.