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arXiv:2606.15292

Light-induced nonadiabatic dissipative quantum dynamics of the Na2 molecule

Patrick Barron, Krisztián Szabó, Gábor J. Halász, Kálmán Varga, Ágnes Vibók

quant-phphysics.atm-clusSubmitted Jun 13, 2026• Announced Jun 16, 2026• Revised Jun 17, 2026 (v2)
v1 · Jun 13, 2026v2 · Jun 17, 2026
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Abstract

Strong light-matter coupling between molecules and optical or plasmonic cavity modes has emerged as a promising platform for advancing photonics, materials science, and chemistry. However, optical cavities and plasmonic resonators in particular are inherently lossy systems characterized by finite photon lifetimes. Accurate theoretical descriptions of molecular dynamics under strong coupling therefore require a proper treatment of cavity losses. In this work, we compare three theoretical approaches for modeling dissipative molecule-cavity dynamics within a realistic parameter regime: the Lindblad master equation, the stochastic Schrödinger equation, and the non-Hermitian Schrödinger equation. As an example, we consider the two lowest energy state of Na2 molecule coupled to a cavity mode and analyze the time evolution of the excited-state population and the mean photon number. Our results demonstrate that the stochastic Schrödinger equation provides an accurate and computationally efficient alternative to the Lindblad master equation, while the non-Hermitian Schrödinger approach is found to be applicable only within a limited range of conditions. Furthermore, we show that inclusion of molecular rotation leads to rotational-vibrational-photonic coupling and gives rise to pronounced nonadiabatic dynamics through light-induced conical intersections. These findings highlight the importance of both dissipation and rotational degrees of freedom for a realistic description of molecular dynamics in strongly coupled molecule-cavity systems.

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Strong light-matter coupling between molecules and optical or plasmonic cavity modes has emerged as a promising platform for advancing photonics, materials science, and chemistry. However, optical cavities and plasmonic resonators in particular are inherently lossy systems characterized by finite photon lifetimes. Accurate theoretical descriptions of molecular dynamics under strong coupling therefore require a proper treatment of cavity losses. In this work, we compare three theoretical approaches for modeling dissipative molecule-cavity dynamics within a realistic parameter regime: the Lindblad master equation, the stochastic Schrödinger equation, and the non-Hermitian Schrödinger equation. As an example, we consider the two lowest energy state of Na2 molecule coupled to a cavity mode and analyze the time evolution of the excited-state population and the mean photon number. Our results demonstrate that the stochastic Schrödinger equation provides an accurate and computationally efficient alternative to the Lindblad master equation, while the non-Hermitian Schrödinger approach is found to be applicable only within a limited range of conditions. Furthermore, we show that inclusion of molecular rotation leads to rotational-vibrational-photonic coupling and gives rise to pronounced nonadiabatic dynamics through light-induced conical intersections. These findings highlight the importance of both dissipation and rotational degrees of freedom for a realistic description of molecular dynamics in strongly coupled molecule-cavity systems.
We address topics related to molecules coupled to quantum radiation. The formalism of light-matter interaction is different for classical and quantum fields, but some analogies remain, such as the formation of light induced crossings. We show that under particular circumstances, the molecular dynamics under quantum or classical fields produce similar results, as long as the radiation is prepared as a Fock state and far from ultra-strong coupling regimes. At this point, the choice of specific initial Fock states is irrelevant since the dynamics scales. However, in realistic multistate molecular systems, radiative scaling may fail due to the presence of simultaneous efficient non-radiative couplings in the dynamics. Polar molecules have permanent dipoles, and within the context of the full quantum Rabi model with a Pauli-Fierz Hamiltonian, they play a crucial role in the polaritonic dynamics since both permanent dipole moments and self-energy terms produce drastic changes on the undressed potential energy surfaces at high coupling strengths. We also gauge the effect of including rotational degrees of freedom in cavity molecular photodynamics. For diatomic molecules, the addition of rotation amounts to transform (both with classical or quantum fields) a light induced crossing into a light induced conical intersection. However, we show that conical intersections due to molecular rotation do not represent the standard properties of well-known efficient intrinsic conical intersections inasmuch they do not enhance the quantum transition rates.
Quantum gases of atoms and molecules in optical cavities offer a formidable laboratory for studying the out-of-equilibrium dynamics of open quantum systems with long-range interactions. Long-range interactions are here mediated by multiple scattering of cavity photons and can induce the formation of quantum structures in space and time. Control of these dynamics requires a detailed understanding of all relevant mechanisms at play. Due to the strong correlations induced by light, however, perturbative theoretical models, which reduce the number of degrees of freedom, do not correctly capture the regime where the interplay of photon-mediated long-range forces and quantum fluctuations of light and matter become significant, such as across the transition to self-organization. In this work, we present the derivation of an effective Lindblad master equation for the dynamics of the sole motional variables of polarizable particles, such as atoms or molecules, that dispersively couple to cavity fields. The master equation is valid even for relatively large intracavity photon numbers and is apt to study both the steady-state regime and the out-of-equilibrium dynamics where quantum fluctuations of the field seed the onset of macroscopic coherences. We validate the theoretical description by showing that it captures the dynamics across a wide temperature interval, from Doppler cooling down to the ultracold regime, and from weak to strong cavity-mediated interactions. Our theory provides a powerful framework for the description of cavity-induced dynamics of quantum matter. In doing so, it permits to connect models of statistical mechanics with cavity-QED experimental platforms, thus enabling quantum simulation of long-range-interacting matter.
Light-matter coupling strength and optical loss are two key physical quantities in cavity quantum electrodynamics (CQED), and their interplay determines whether light-matter hybrid states can be formed or not in chemical systems. In this study, by using macroscopic quantum electrodynamics (MQED) combined with a pseudomode approach, we present a simple but accurate method, which allows us to quickly estimate the light-matter coupling strength and optical loss without free parameters. Moreover, for a molecular emitter coupled with photonic modes (including cavity modes and plasmon polariton modes), we analytically and numerically prove that the dynamics derived from the MQED-based wavefunction approach is mathematically equivalent to the dynamics governed by the CQED-based Lindblad master equation when the Purcell factor behaves like Lorentzian functions.
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.
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.
Room-temperature cavity quantum electrodynamics with molecular materials in optical cavities offers exciting prospects for controlling electronic, nuclear and photonic degrees of freedom for applications in physics, chemistry and materials science. However, achieving strong coupling with molecular ensembles typically requires high molecular densities and substantial electromagnetic-field confinement. These conditions usually involve a significant degree of molecular disorder and a highly structured photonic density of states. It remains unclear to what extent these additional complexities modify the usual physical picture of strong coupling developed for atoms and inorganic semiconductors. Using a microscopic quantum description of molecular ensembles in realistic multimode optical resonators, we show that the emergence of vacuum Rabi splitting in linear spectroscopy is a necessary but not sufficient metric of coherent admixing between light and matter. In low-finesse multi-mode situations, we find that molecular dipoles can be partially hybridized with photonic dissipation channels associated with off-resonant cavity modes. These vacuum-induced dissipative processes ultimately limit the extent of light-matter coherence that the system can sustain.This article is part of the theme issue 'The quantum theory of light'.