Phenomenological approaches to photon loss have long been the workhorse of cavity-QED, but prove inadequate in the presence of sufficiently broadband light-matter interactions. We present a rigorous and ab initio derivation of a quantum master equation for a quantized optical cavity mode coupled to a dipole, using a quasinormal mode (QNM) quantization procedure for plasmonic and dielectric open-system cavity-QED, which is valid in broadband light-matter interaction regimes, including ultrastrong coupling (USC). The theory supports general three-dimensional resonators with arbitrary dispersion and loss, and thus can be applied to a wide range of realistic open cavities. Our ab initio and gauge-invariant approach fully recovers a recent result for the spectral density of a quantized cavity with a single dipole and reveals important departures from previous heuristic assumptions about system-reservoir coupling. We identify a new criterion for what we term the "broadband dissipative" regime of cavity-QED, where phenomenological models require corrections in accordance with the intrinsic and spatially-dependent complex phase of the QNM, and also shed light on fundamental limits to single-mode models in extreme coupling regimes. Using experimentally motivated plasmonic and dielectric cavity examples, we show validity ranges of our QNM master equation and spectral USC calculations, and discuss prospects for near-term experimental observation of the broadband dissipative effects.
Phenomenological approaches to photon loss have long been the workhorse of cavity-QED, but prove inadequate in the presence of sufficiently broadband light-matter interactions. We present a rigorous and ab initio derivation of a quantum master equation for a quantized optical cavity mode coupled to a dipole, using a quasinormal mode (QNM) quantization procedure for plasmonic and dielectric open-system cavity-QED, which is valid in broadband light-matter interaction regimes, including ultrastrong coupling (USC). The theory supports general three-dimensional resonators with arbitrary dispersion and loss, and thus can be applied to a wide range of realistic open cavities. Our ab initio and gauge-invariant approach fully recovers a recent result for the spectral density of a quantized cavity with a single dipole and reveals important departures from previous heuristic assumptions about system-reservoir coupling. We identify a new criterion for what we term the "broadband dissipative" regime of cavity-QED, where phenomenological models require corrections in accordance with the intrinsic and spatially-dependent complex phase of the QNM, and also shed light on fundamental limits to single-mode models in extreme coupling regimes. Using experimentally motivated plasmonic and dielectric cavity examples, we show validity ranges of our QNM master equation and spectral USC calculations, and discuss prospects for near-term experimental observation of the broadband dissipative effects.
The unprecedented pace of evolution in nanoscale architectures for cavity quantum electrodynamics (cQED) has posed crucial challenges for theory, where the quantum dynamics arising from the non-perturbative dressing of matter by cavity electric and magnetic fields as well as the fundamentally non-Hermitian character of the system are to be treated without significant approximation. The lossy electromagnetic resonances of photonic, plasmonic, or magnonic nanostructures are described as quasinormal modes (QNMs), whose properties and interactions with quantum emitters and spin qubits are central to the understanding of dissipative nano-optics and magnetodielectric cQED. Despite recent advancements toward a fully quantum framework for QNMs, a general and universally accepted approach to QNM quantization for arbitrary linear media remains elusive. In this work, we introduce a unified theoretical framework, based on macroscopic QED and complex coordinate transformations, which achieves QNM quantization for a wide class of spatially inhomogeneous, dissipative and dispersive, linear, magnetodielectric resonators. The complex coordinate transformations equivalently convert the radiative losses into non-radiative material dissipation, and via a suitable transformation that reflects all the losses of the resonator, we define creation and annihilation operators that allow the construction of modal Fock states for the joint excitations of field-dressed matter. By directly addressing the intricacies of modal loss in a fully quantum theory of magnetodielectric cQED, our approach enables the exploration of modern, quantum nano-optical experiments utilizing dielectric, plasmonic, magnetic, or hybrid cQED architectures and paves the way toward a rigorous assessment of room-temperature, quantum nanophotonic technologies without recourse to ad hoc quantization schemes.
In the presence of arbitrary three-dimensional linear media with material loss and amplification, we present an electromagnetic field quantization scheme for quasinormal modes (QNMs), extending previous work for lossy media [S. Franke et al., Phys. Rev. Lett. 122, 213901 (2019)]. Applying a symmetrization transformation, we show two fundamentally different ways for constructing a QNM photon Fock space, including (i) where there is a separate operator basis for both gain and loss, and (ii) where the loss and gain degrees of freedom are combined into a single basis. These QNM operator bases are subsequently used to derive the associated QNM master equations, including the interaction with a quantum emitter, modeled as a quantized two-level system (TLS). We then compare the two different quantization approaches, and also show how commonly used phenomenological methods to quantize light in gain-loss resonators are corrected by several important aspects, such as a loss-induced and gain-induced intermode coupling, which appears through the rigorous treatment of loss and amplification on a dissipative mode level. For specific resonator designs, modeled in a fully consistent way with the classical Maxwell equations with open boundary conditions, we then present numerical results for the quantum parameters and observables of a TLS weakly interacting with the medium-assisted field in a gain-loss microdisk resonator system, and discuss the validity of the different quantization approaches for several gain-loss parameter regimes.
Devices involving bound or propagating photons are among the basic building blocks for modern quantum technologies. For example, the bound modes of open optical resonators, coupled to quantum emitters such as atoms, molecules, or quantum dots, are used for an enhanced emission in lasing applications, for increased sensitivity in quantum sensing, and as qubits in quantum computing. Meanwhile, propagating photons are crucial for the transmission of quantum states between spatially separated systems. In this thesis, we develop a rigorous theory of multiple, spatially separated, and individually addressable cavities (or plasmonic resonators) for applications in modern quantum devices. Losses are modeled via the use of quasinormal modes (QNMs), which are solutions to the source-free Helmholtz equation under open boundary conditions, making them the natural modes of open resonators. Quantum emitters are modeled as two-level systems (TLSs) which couple to the electric field via dipole coupling. The multi-cavity theory is developed in three steps: 1. We present a classical scattering theory for a system of multiple QNM cavities, where the multi-cavity Green's function is formulated in terms of the single-cavity modes. The inter-cavity scattering is frequency-dependent to account for retardation delays, and is efficiently calculated numerically, using common (commercial) solvers. 2. We formulate a quantization scheme for QNMs of spatially separated open resonators. We introduce the \textit{cavity separation parameter} as a simple measure for when QNM cavities can be quantized separately and when they have to be treated as a single system with a joint set of operators. We derive a general system-bath Hamiltonian that contains coupling between bound modes, quantum emitters, and a bath of propagating photons, expressed via rigorous, numerically calculable coupling parameters. 3. We discuss the time-dependent theory of QNMs and TLSs coupled to propagating photons. The system-bath interaction is formulated in terms of correlation functions that are again rigorously defined in terms of numerically calculable QNM parameters. The correlation functions are immediately applicable to common methods for calculating the dynamics of open quantum systems. Steps 1-3 are all formulated for general cavity shapes and materials, as well as (in principle) arbitrary background structures. Hence, the theory is applicable to a wide range of devices, including cavities or plasmonic resonators in free space, on a photonic crystal, or on a substrate. For each step, we show example calculations for one-dimensional or three-dimensional cavities.
Cavity Quantum Electrodynamics (Cavity-QED) offers a powerful framework for controlling light-matter interactions, yet first-principles approaches commonly assume ideal, lossless cavity fields. Here, we introduce a minimal extension to the Pauli-Fierz Hamiltonian that accounts for cavity dissipation through the experimentally accessible cavity quality factor Q. The electromagnetic field is described as a damped harmonic oscillator within the very weak damping approximation. In this framework, cavity losses only enter the light-matter interaction and dipole self-energy terms, without introducing additional photonic degrees of freedom. A time-dependent unitary transformation yields a real-valued Hermitian Hamiltonian that can be incorporated into existing ab-initio QED methods without additional computational cost or changes in scaling. We combined the approach to the QED-CCSD method and investigated the effects of cavity dissipation on the optical spectrum of a p-nitroaniline molecule under strong light-matter coupling. We found that, for realistic quality factors, cavity dissipation can reduce the Rabi splitting by more than 20% compared to the ideal-cavity limit, even though the system remains in the strong-coupling regime. Convergence towards the ideal-cavity limit then requires substantially higher quality factors than those needed to establish strong coupling. These results demonstrate that cavity dissipation can significantly affect polaritonic energetics and highlight the importance of incorporating experimentally realistic cavity losses into quantitative ab-initio Cavity-QED simulations to accurately guide experimental protocols.
We introduce a second quantization scheme based on quasinormal modes, which are the dissipative modes of leaky optical cavities and plasmonic resonators with complex eigenfrequencies. The theory enables the construction of multiplasmon or multiphoton Fock states for arbitrary three-dimensional dissipative resonators and gives a solid understanding to the limits of phenomenological dissipative Jaynes-Cummings models. In the general case, we show how different quasinormal modes interfere through an off-diagonal mode coupling and demonstrate how these results affect cavity-modified spontaneous emission. To illustrate the practical application of the theory, we show examples using a gold nanorod dimer and a hybrid dielectric-metal cavity structure.
Strong periodic driving of cavity-quantum electrodynamics (QED) in the ultrastrong-coupling regime creates nonequilibrium states whose dissipation is governed by Floquet quasienergies rather than undriven dressed resonances. However, modeling such a regime is a significant theoretical challenge, including a number of subtle problems such as the need to ensure gauge invariance for truncated matter-cavity systems with time-dependent driving. To fill this theoretical gap, we introduce a nonsecular Floquet generalized master equation framework for strongly driven open cavity-QED systems, formulated in the dressed basis of the quantum Rabi model and applicable to structured reservoirs without rotating-wave approximations. Our theory can thus model Floquet-driven dynamics in open ultrastrong-coupling cavity-QED, and demonstrates a wide range of quantum state control. Using strong optical pumping and parametric mechanical modulation, we compute long-time populations, fluorescence spectra, and the Floquet-Liouville eigenspectra, resolving observable resonances into hybridized quasienergy channels and decay rates. By systematically comparing with conventional time-independent dressed-basis generalized master equations, we show that static approaches only reproduce steady-state populations in restricted excitation regimes, and fail for frequency-resolved observables and break down under appropriate Floquet engineering, surprisingly, even for spectrally flat baths. Structured environments, such as Lorentzian-Ohmic reservoirs, further amplify these discrepancies through sideband-selective decay. Our results demonstrate that dissipation in driven ultrastrong cavity-QED is intrinsically quasienergy resolved and we establish Floquet-dissipative theory as an accurate and powerful framework for predicting spectra, controlling decay pathways, and engineering nonequilibrium quantum states and reservoirs.