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The Journal of Chemical Physics

Dynamics of disordered Tavis–Cummings and Holstein–Tavis–Cummings models

Kewei Sun, Cunzhi Dou, Maxim F. Gelin, Yang Zhao

Published Dec 21, 2021• 44 citations
Publisher

Abstract

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.

DOI
10.1063/5.0076485

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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.
By employing the numerically accurate multiple Davydov Ansatz (mDA) formalism in combination with the thermo-field dynamics (TFD) representation of quantum mechanics, we systematically explore the influence of three parameters-temperature, photonic-mode detuning, and qubit-phonon coupling-on population dynamics and absorption spectra of the Holstein-Tavis-Cummings (HTC) model. It is found that elevated qubit-phonon couplings and/or temperatures have a similar impact on all dynamic observables: they suppress the amplitudes of Rabi oscillations in photonic populations as well as broaden the peaks and decrease their intensities in the absorption spectra. Our results unequivocally demonstrate that the HTC dynamics is very sensitive to the concerted variation of the three aforementioned parameters, and this finding can be used for fine-tuning polaritonic transport. The developed mDA-TFD methodology can be efficiently applied for modeling, predicting, optimizing, and comprehensively understanding dynamic and spectroscopic responses of actual molecular systems in microcavities.
N\mathcal{N}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.
We present a comprehensive theoretical and computational study of the Tavis–Cummings model in the collective-spin basis, addressing both its static spectral properties and dynamic behavior under unitary and open-system evolution. By exploiting the commutation of the total-excitation operator with the Hamiltonian, we construct block-diagonal representations for systems of two-level molecules coupled to a single quantized cavity mode. We derive analytic expressions for the degeneracies, block dimensions, and secular polynomials, introducing a family of orthogonal “Félix–Sanz-Vicario” new class of orthogonal polynomials (here baptized Félix-Sanz-Vicario polynomials) whose roots furnish the energy eigenvalues and whose finite-degree structure allows precise control over photon-number truncation in small manifolds. Numerical implementations in Python (QuTiP) confirm exact agreement with the original Tavis–Cummings solution in each excitation manifold, while also highlighting the role of lower-spin subspaces—absent in the bosonized highest-spin description—in mediating configurational molecular interactions via a rank-1 spherical tensor operator. Time-dependent simulations compare dynamics under the rotating wave aproximation (Tavis-Cummings model) and without it (Dicke model), demonstrating population transfer, Rabi oscillations, and collapse–revival phenomena. The dynamics of open quantum system, via a Lindblad master equation, illustrate cavity-loss effects on photon-number decay, von Neumann entanglement entropy, and coherent exchange under dissipation. Our results establish that the collective-spin framework, using a set of solutions in terms of orthogonal polynomials, provides both analytical insight and computational efficiency for spectroscopic modeling, ultrastrong coupling studies, and the design of low-photon-number quantum simulations.
We examine the applicability of the numerically accurate method of time dependent variation with multiple Davydov Ansätze (mDA) to non-Hermitian systems. As illustrative examples, three systems of interest have been studied, a non-Hermitian system of dissipative Landau-Zener transitions, a non-Hermitian multimode Jaynes-Cummings model, and a dissipative Holstein-Tavis-Cummings model, all of which are shown to be effectively described by the mDA method. Our findings highlight the versatility of the mDA as a powerful numerical tool for investigating complex many-body non-Hermitian systems, which can be extended to explore diverse phenomena such as skin effects, excited-state dynamics, and spectral topology in the non-Hermitian field.
This work investigates the emergent thermalization regimes in a chaotic Tavis-Cummings (TC) model and their implications in quantum spectroscopy. While the TC model is a cornerstone of cavity quantum electrodynamics, traditional treatments often overlook many-body effects that arise in the thermodynamic limit. We utilize the Eigenstate Thermalization Hypothesis to demonstrate that a non-integrable excitonic Hamiltonian within the material manifold drives local thermalization. By tuning the polariton splitting ggg, we observe two dynamical regimes: a thermalizing regime at low interactions driven by quantum chaos and ergodicity, and a non-thermalizing regime at high interactions where strong coupling suppresses ergodicity. We further show that these regimes have direct implications on output photon statistics, specifically influencing the correlation times τcτ_cτc​ of the cavity population and the second-order correlation function g(2)(t+τ)g^{(2)}(t+τ)g(2)(t+τ). We propose that entangled-biphoton spectroscopy serves as an ideal experimental platform to probe these effects and to allow the characterization of the underlying many-body exciton-coupling disorder σσσ through coincidence measurements of the output. Taken together, these results exploit a naturally occurring many-body phenomenon to bridge theoretical predictions with experimental observables.
We employed the Tavis-Cummings model to study the pump-probe spectra of molecular polaritons. To describe the dissipative effects caused by the environment, the population decays of the photon mode and the two level states (TLSs), as well as the fast component of the dephasing of TLSs, are described by using the Lindblad equation. The effect of static disorder in the TLS transition frequency is incorporated into the equation of motion of the density matrix. The pump-probe spectra of the model system are calculated using the optical response function approach. Pronounced Rabi oscillations are observed in the pump-probe spectra, which are signatures of the strong light-matter coupling between the cavity mode and the collective bright state of the TLSs. To help understand the pump-probe spectra, we also simulate the laser pulse induced dynamics of the bright state of the molecular polaritons. The results show that the bright state lifetime is primarily determined by the dephasing time of the TLSs, consistent with the fast decay of the Rabi oscillations observed in the pump-probe spectra. Once the coherence decays, the long-time pump-probe response is dominated by the excited state population of the dark state manifold.