$\mathcal{N}$ emitters collectively coupled to a quantized cavity mode are described by the Tavis-Cummings model. We present a complete analytical solution of the model in the presence of inhomogeneous couplings and energetic disorder. We derive the exact expressions for the bright and the dark sectors that decouple the disordered model and find that, in the thermodynamic limit, the energetic disorder transforms the bright sector to Fano's model that can be easily solved. We thoroughly explore the effects of energetic disorder assuming a Gaussian distribution of emitter transition energies. We compare the Fano resonances in optical absorption and inelastic electron scattering in both the weak and the strong coupling regimes. We study the evolution of the optical absorption with an increase in the disorder strength and find that it changes the lower and upper polaritons to their broadened resonances that finally transform to a single resonance at the bare cavity photon energy, thus taking the system from the strong to the weak coupling regime. Interestingly, we learn that Rabi splitting can exist even in the weak coupling regime, while the polaritonic peaks in the strong coupling regime can represent almost excitonic states at intermediate disorder strengths. We also calculate the photon Green's function to see the effect of cavity leakage and nonradiative emitter losses and find that the polariton line width exhibits a minimum as a function of detuning when the cavity leakage is comparable to the Fano broadening.
N emitters collectively coupled to a quantized cavity mode are described by the Tavis-Cummings model. We present a complete analytical solution of the model in the presence of inhomogeneous couplings and energetic disorder. We derive the exact expressions for the bright and the dark sectors that decouple the disordered model and find that, in the thermodynamic limit, the energetic disorder transforms the bright sector to Fano's model that can be easily solved. We thoroughly explore the effects of energetic disorder assuming a Gaussian distribution of emitter transition energies. We compare the Fano resonances in optical absorption and inelastic electron scattering in both the weak and the strong coupling regimes. We study the evolution of the optical absorption with an increase in the disorder strength and find that it changes the lower and upper polaritons to their broadened resonances that finally transform to a single resonance at the bare cavity photon energy, thus taking the system from the strong to the weak coupling regime. Interestingly, we learn that Rabi splitting can exist even in the weak coupling regime, while the polaritonic peaks in the strong coupling regime can represent almost excitonic states at intermediate disorder strengths. We also calculate the photon Green's function to see the effect of cavity leakage and nonradiative emitter losses and find that the polariton line width exhibits a minimum as a function of detuning when the cavity leakage is comparable to the Fano broadening.
Davydov trial states, in combination with the Green's function method, we study the dynamics of the Tavis-Cummings model and the Holstein-Tavis-Cummings model in the presence of diagonal disorder and cavity-qubit coupling disorder. For the Tavis-Cummings model, time evolution of the photon population, the optical absorption spectra, and the hetero-entanglement between the qubits and the cavity mode are calculated by using the Green's function method to corroborate numerically exact results of Davydov's Ansätze. For the Holstein-Tavis-Cummings model, only the latter is utilized to simulate effects of disorder on the photon population dynamics and the absorption spectra. We have demonstrated that the complementary employment of analytical and numerical methods permits uncovering a fairly comprehensive picture of a variety of complex behaviors in disordered multidimensional polaritonic cavity quantum electrodynamics systems.
The interaction of an ensemble of N 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=Ng1, where g1 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.
The Tavis-Cummings model is a paradigmatic central-mode model in which a set of two-level quantum emitters (spins) are coupled to a collective cavity mode. Here we study the eigenstate spectrum, its localization properties, and the effect on dynamics, focusing on the two-excitation sector relevant for nonlinear photonics. These models admit two sources of disorder: in the coupling between the spins and the cavity, and in the energy shifts of the individual spins. While this model was known to be exactly solvable in the limit of a homogeneous coupling and inhomogeneous energy shifts, we establish here the solvability in the opposite limit of a homogeneous energy shift and inhomogeneous coupling, presenting the exact solution and corresponding conserved quantities. We identify three different classes of eigenstates, exhibiting different degrees of multifractality and semilocalization closely tied to the integrable points, and we study their stability to perturbations away from these solvable points. The dynamics of the cavity occupation number away from equilibrium, exhibiting boson bunching and a two-photon blockade, is explicitly related to the localization properties of the eigenstates, and it illustrates how these models support a collective spin description despite the presence of disorder. Published by the American Physical Society 2024
An empirical framework for studying the way vacuum fluctuations in a Fabry–Perot cavity produce collective light–matter hybrid states (polariton states) is reported. The reason that the Tavis–Cummings model, where a single mode of the radiation field couples to all the molecules, succeeds is discussed in terms of the strong phase correlation of the vacuum fluctuations in the cavity, which produces a single effective cavity mode (ECM). The model is used to study the onset of the collective state, or “superradiant phase”, for ensembles of molecules with significant disorder in their transition energies, as a function of cavity strength factor, from low Q cavities to high Q cavities. A key result is the quantification of the coherence of the ensemble of the lowest energy eigenstate. This is assessed, primarily, using an entropy distance measure. The statistical model provides a physical intuition for the formation of coherence of polariton states when the collective coupling is strong enough that they dominate over the tail of the dark-state density-of-states.
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.
We analyze vibrational dynamics in a toy model for polaritonic chemistry under collective electronic strong coupling. In a Holstein-Tavis-Cummings model, incoherently excited by a photon, we show that disorder leads to non-Gaussian states of vibrational modes on short time scales at the single-molecule level. Using exact matrix product state simulations, we demonstrate that this effect can remain robust for larger molecule numbers, implying that nuclear wave packets cannot be effectively described by thermal states. Furthermore, we compare simulations of the exact quantum dynamics with semiclassical approximations. We find that the Ehrenfest approximation can only well reproduce ensemble-averaged observables for very large system sizes. Also simulations in the truncated Wigner approximation fail to capture the non-Gaussian effects. Our work highlights the importance of disorder and genuine quantum effects in cavity-modified nuclear dynamics in polaritonic chemistry.