Strong light-matter interactions in optical microcavities give rise to hybrid light-matter states known as polaritons. While actively used in modern technologies, theoretical descriptions of such systems are often restricted to the single-excitation case, limiting their ability to capture many-excitation physics and hindering further technological advancements. Here, by exploiting the combinatorial structure of quantum emitters, we investigate the Tavis-Cummings model with arbitrary number of excitations. We derive the structure and properties of its eigensystem and identify allowed radiative transitions in systems of realistic size scales. Our work reveals new behavior inaccessible to the few-excitation regime, while also providing a framework to reduce the computational complexity of similar systems with exponentially growing Hilbert spaces.
Strong light-matter interactions in optical microcavities give rise to hybrid light-matter states known as polaritons. While actively used in modern technologies, theoretical descriptions of such systems are often restricted to the single-excitation case, limiting their ability to capture many-excitation physics and hindering further technological advancements. Here, by exploiting the combinatorial structure of quantum emitters, we investigate the Tavis-Cummings model with arbitrary number of excitations. We derive the structure and properties of its eigensystem and identify allowed radiative transitions in systems of realistic size scales. Our work reveals new behavior inaccessible to the few-excitation regime, while also providing a framework to reduce the computational complexity of similar systems with exponentially growing Hilbert spaces.
Confined electromagnetic modes strongly couple to collective excitations in ensembles of quantum emitters, producing light–matter hybrid states known as polaritons. Under such conditions, the discrete multilevel spectrum of molecular systems offers an appealing playground for exploring multiphoton processes. This work contrasts predictions from the Tavis–Cummings model in which the material is a collection of two-level systems, with the implications of considering additional energy levels with harmonic and anharmonic structures. We discuss the exact eigenspectrum, up to the second excitation manifold, of an arbitrary number N of oscillators collectively coupled to a single cavity mode in the rotating-wave approximation. Elaborating on our group-theoretic approach [New J. Phys. 23, 063081 (2021)], we simplify the brute-force diagonalization of N2 × N2 Hamiltonians to the eigendecomposition of, at most, 4 × 4 matrices for arbitrary N. We thoroughly discuss the eigenstates and the consequences of weak and strong anharmonicities. Furthermore, we find resonant conditions between bipolaritons and anharmonic transitions where two-photon absorption can be enhanced. Finally, we conclude that energy shifts in the polaritonic states induced by anharmonicities become negligible for large N. Thus, calculations with a single or few quantum emitters qualitatively fail to represent the nonlinear optical response of the collective strong coupling regime. Our work highlights the rich physics of multilevel anharmonic systems coupled to cavities absent in standard models of quantum optics. We also provide concise tabulated expressions for eigenfrequencies and transition amplitudes, which should serve as a reference for future spectroscopic studies of molecular polaritons.
The enormous progress in controlling quantum optical and atomic systems has prompted ideas for new experimental realizations of strongly correlated many-body systems operating with light. These systems consist of photons confined in optical cavities, which interact strongly with atoms or atomiclike structures. Due to the interaction between the two particle species optical nonlinearities appear, leading to a quantum phase transition from Mott to superfluid phase. Here, we address the Tavis-Cummings lattice model, which describes light-matter systems containing multiple atomiclike structures in each cavity. In particular, we investigate the phase boundary delimiting Mott from superfluid phase and the elementary excitations of the two-dimensional Tavis-Cummings lattice model in dependence of the number of atomiclike structures per cavity. In order to obtain the results we employ the variational cluster approach. We evaluate spectral functions and densities of states of both particle species, which allows us to characterize the fundamental excitations of light-matter systems. These excitations are termed polaritons and are superpositions of photons and atomic excitations. We introduce polariton quasiparticles as appropriate linear combinations of both particle species and analyze the weights of their constituents. Our results demonstrate the dependence of the quantum phase transition and the elementary excitations on the number of atomiclike structures per cavity and provide thus valuable insight into the physics of light-matter systems.
Strong light-matter coupling gives rise to polaritons - hybrid excitations whose mixed photonic and matter character enables control over optical, electronic and chemical properties. This Feature Article surveys the main architectures supporting polariton formation, including photonic microcavities, plasmonic nanostructures, open cavities and metasurfaces, and outlines how inorganic semiconductors, organic aggregates and hybrid systems access strong and ultrastrong coupling. Key phenomena such as coherent dynamics, vibronic interactions, dark-state reservoirs and polariton-mediated energy and electron transport are discussed, together with the experimental and theoretical tools used to study them. We highlight examples where strong coupling modifies charge transport, energy flow and chemical reactivity, and we summarize emerging regimes, including intermediate and dark-strong coupling, that broaden the landscape of hybrid light-matter physics.
Abstract The interaction between anharmonic quantum emitters (e.g. molecular vibrations) and confined electromagnetic fields gives rise to quantum states with optical and chemical properties that are different from those of their precursors. The exploration of these properties has been typically constrained to the first excitation manifold, the harmonic approximation, ensembles of two-level systems [Tavis–Cummings (TC) model], or the anharmonic single-molecule case. The present work studies, for the first time, a collective ensemble of identical multi-level anharmonic emitters and their dipolar interaction with a photonic cavity mode, which is an exactly solvable many-body problem. The permutational properties of the system allow identifying symmetry classified submanifolds in the energy spectrum. Notably, in this approach, the number of particles, typically in the order of several millions, becomes only a parameter from the operational standpoint, and the size of the dimension of the matrices to diagonalize is independent of it. The formalism capabilities are illustrated by showing the energy spectrum structure, up to the third excitation manifold, and the calculation of the photon contents as a permutationally invariant quantity. Emphasis is placed on (a) the collective (superradiant) scalings of light–matter couplings and the various submanifolds of dark (subradiant) states with no counterpart in the single-molecule case, as well as (b) the delocalized modes containing more than one excitation per molecule with no equivalent in the TC model. We expect these findings to be applicable in the study of non-linear spectroscopy and chemistry of polaritons.
We present a systematic study of the properties of systems composed of N two-level quantum emitters coupled to a single cavity mode, for light-matter interaction strengths ranging from the weak to the ultrastrong and deep-strong coupling regimes. Beginning with an analysis of the energy spectrum as a function of the light-matter coupling strength, we examine systems with varying numbers of emitters, from a pair to large collections, approaching the thermodynamic limit $(N\ensuremath{\rightarrow}\ensuremath{\infty})$. Additionally, we explore the emission properties of these systems under incoherent excitation of the emitters, employing a general theoretical framework for open cavity-QED systems, which is valid across all light-matter interaction regimes and preserves gauge invariance within truncated Hilbert spaces. Furthermore, we study the influence of the emitter-environment interaction on the spectral properties of the system. Specifically, when each emitter interacts independently with its own reservoir, we observe the emergence of an emission peak at the cavity's resonant frequency for even values of N. Our analysis also clarifies the evolution of the system as the number of emitters increases, ultimately converging toward an equivalent system composed of two interacting single-mode bosonic fields.
The field of Polaritonic Chemistry studies molecules strongly coupled to the light field of optical cavities. The resulting modification of the potential energy landscape has been demonstrated to enable control over the chemical and physical properties of materials and molecular ensembles. This thesis extends the Tavis–Cummings model to describe molecules under strong light–matter coupling, incorporating static dipole moments and dipole self-energy contributions derived from the Pauli–Fierz Hamiltonian. These additional terms are shown to be essential for reproducing cavity-modified molecular dynamics and spectra. Simulations on the nuclear wavefunction propagation of MgH+ molecules demonstrate the impact of these terms, while an effective two-level system model accurately captures the behavior of large ensembles. Beyond single excitations, the thesis also explores the higher excitation manifolds of the Tavis-Cummings model, which reveals that allowing for more than a single excitation makes the reaction of the involved polaritons entropically more favorable. Open-system simulations highlight how the coherence of the system's initial state governs decay pathways and enables long-lived energy storage. Finally, a multilevel vibrational model coupled to a two-mode cavity is introduced, where a Raman scheme enables selective mixing of vibrational states. The simulation results show that continuous pumping can drive molecules into specific vibrational states while suppressing electronic excitation, both for single molecules and small ensembles. Together, these results provide new theoretical insights into the mechanisms by which optical cavities reshape molecular energy landscapes. The results suggest approaches for controlling photonic, electronic, and vibrational dynamics in strongly coupled systems, contributing to the theoretical foundation of polariton chemistry.