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arXiv:2609.23295

Non-Markovian Quantum Dynamics of Exciton-Polaritons

Rajanya Sarkar, Pritha Ghosh, Arshath Manjalingal, David R. Reichman, Arkajit Mandal

cond-mat.mes-hallcond-mat.mtrl-sciquant-phSubmitted Sep 20, 2026• Announced Sep 22, 2026
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Abstract

Exciton-polaritons, hybrid light-matter quasiparticles formed when a material interacts with a confined electric field, have experimentally been shown to exhibit mesoscale coherent quantum propagation that remains robust at room temperature. However, an accurate and direct quantum dynamical simulation of this phenomenon that does not resort to semi-classical approximations is prohibitively expensive computationally, limiting the microscopic understanding of the rich dynamical interplay among phonons, photons, and electrons under collective light-matter coupling. To address this fundamental challenge, we develop a non-Markovian master equation approach which enables the fully quantum mechanical simulation of non-equilibrium exciton-polariton dynamics and captures phonon-induced decoherence and dissipation beyond the conventional Markovian limit. To carry out this task, a procedure is developed in which the wave vector space is coarse-grained and each diagonal element of the density matrix is evolved in parallel. To demonstrate the utility of this approach, we simulate exciton-polariton transport in TIPS-pentacene. We find that our approach reasonably captures the experimentally observed renormalization of the polariton group velocity, which originates from the phonon-induced non-Markovian Lamb shift. We further show that this renormalization cannot be reproduced within conventional Markovian theories.

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Exciton-polaritons, hybrid light-matter quasiparticles formed when a material interacts with a confined electric field, have experimentally been shown to exhibit mesoscale coherent quantum propagation that remains robust at room temperature. However, an accurate and direct quantum dynamical simulation of this phenomenon that does not resort to semi-classical approximations is prohibitively expensive computationally, limiting the microscopic understanding of the rich dynamical interplay among phonons, photons, and electrons under collective light-matter coupling. To address this fundamental challenge, we develop a non-Markovian master equation approach which enables the fully quantum mechanical simulation of non-equilibrium exciton-polariton dynamics and captures phonon-induced decoherence and dissipation beyond the conventional Markovian limit. To carry out this task, a procedure is developed in which the wave vector space is coarse-grained and each diagonal element of the density matrix is evolved in parallel. To demonstrate the utility of this approach, we simulate exciton-polariton transport in TIPS-pentacene. We find that our approach reasonably captures the experimentally observed renormalization of the polariton group velocity, which originates from the phonon-induced non-Markovian Lamb shift. We further show that this renormalization cannot be reproduced within conventional Markovian theories.
Exciton-polaritons are light-matter hybrid quasi-particles that have emerged as a flexible platform for developing quantum technologies and engineering material properties. However, the fundamental mechanistic principles that govern their dynamics and relaxation remain elusive. In this work, we provide the microscopic mechanistic understanding of the exciton-polariton relaxation process that follows from an excitation in the upper polariton. Using both mixed quantum-classical simulations and analytical analysis, we reveal that phonon-induced upper-to-lower polariton relaxation proceeds via two steps: the first step is a vertical inter-band transition from the upper to the lower polariton, which is followed by a second step that is a phonon-induced Fröhlich scattering within the lower polariton. We find that in materials of finite thickness (which include filled cavities), phonon-induced polaritonic intraband Fröhlich scattering is significantly suppressed. We show that the microscopic origin of this suppression is phonon-fluctuations synchronization (or self-averaging) due to the polaritonic spatial delocalization in the quantization direction. Finally, we show that the same phonon fluctuation-synchronization effect plays a central role across polaritonic relaxation pathways, and we derive simple analytical expressions that relate a material's finite thickness to the corresponding relaxation rate constants.
Understanding how strong correlations and dissipation combine to shape collective quantum excitations is a central challenge in many-body physics. We investigate the effect of dissipative light-matter coupling on strongly interacting exciton-polaritons in the presence of a biexciton resonance, which gives rise to polaron-polariton quasiparticles. We show that the interplay between many-body correlations and non-Hermitian coupling generates anomalous dispersion relations and exceptional points in the polaron-polariton spectrum. The location and coexistence of exceptional points are controlled by the dissipative coupling and the relative decay rates of the excitonic and photonic constituents, allowing them to emerge across different polaron-polariton branches. These results identify dissipative polaron-polaritons as a versatile platform for exploring non-Hermitian many-body physics with tunable light-matter quasiparticles.
Understanding the dynamics of open quantum systems in strong coupling and non-Markovian regimes remains a formidable theoretical challenge. One popular and well-established method of approximation in these circumstances is provided by the polaron master equation (PME). In this work, we re-evaluate and extend the validity of the PME to capture the impact of non-Markovian polaron dressing, induced by non-equilibrium open system dynamics. By comparing with numerically exact techniques, we confirm that while the standard PME successfully predicts the dynamics of system observables that commute with the polaron transformation (e.g., populations in the Pauli z-basis), it can struggle to fully capture those that do not (e.g., coherences). This limitation stems from the mixing of system and environment degrees of freedom inherent to the polaron transformation, which affects the accuracy of calculated expectation values within the polaron frame. Employing the Nakajima-Zwanzig projection operator formalism, we introduce correction terms that provide an accurate description of observables that do not commute with the transformation. We demonstrate the significance of the correction terms in two cases, the canonical spin-boson model and a dissipative time-dependent Landau-Zener protocol, where they are shown to impact the system dynamics on both short and long timescales.
Qubit coherence is an essential figure of merit for quantum information processing applications such as quantum computing, or quantum repeaters. Understanding the coherence properties of the underlying physical qubits that facilitate such applications is therefore are often limited by coupling to lattice phonons, which in turn constrains operation temperature. Here we study phonon induced electronic spin decoherence in group-IV vacancy centers in diamond. We begin by modeling the spin-phonon interaction and then employ the widely used Born-Markov approximation, highlighting its inconsistencies in this setting and its deviations from experimental observations. To close the gap between theoretical predictions and experimental results, we relax certain approximations, investigate their contributions to the predicted coherence times, and identify the dominant sources of discrepancy. We further demonstrate that experimentally measured electronic spin coherence dynamics are consistently captured within a non-Markovian framework, and we show how the magnetic field orientation influences the qubit coherence time.
Development of spontaneous coherence is one of the hallmarks of bosonic condensation in a variety of physical systems, such as cold atoms, confined photons, and hybrid light-matter quasiparticles like exciton polaritons in semiconductors. While spatial coherence is well understood once a steady-state condensate has been established, its temporal evolution as the condensate forms is largely unexplored. Here, we explore the dynamical formation of a non-equilibrium, driven-dissipative exciton-polariton condensate through both time-resolved experiments and numerical modeling. Our study reveals that the spatial coherence is established through two distinct stages. The early-time stage is interaction-driven and features transient oscillations in spatial coherence. This stage is followed by a steady-state regime characterized by a spatially-uniform high degree of coherence that extends over the entire size of the system and persists over time. These stages of spatial coherence development occur in both free flowing and confined exciton-polariton systems that undergo a quench - rapid growth of the condensate starting from two different initial settings. Our study offers a deep insight into the process by which long-range spatial coherence is established in a non-equilibrium bosonic condensate.
Recent advances in quantum technologies and related experiments have created a need for highly accurate, versatile, and computationally efficient simulation techniques for the dynamics of open quantum systems. Long-lived correlation effects (non-Markovianity), system-environment hybridization, and the necessity for accuracy beyond the Born-Markov approximation form particular challenges. Approaches to meet these challenges have been introduced, originating from different fields, such as hierarchical equations of motion, Lindblad-pseudomode formulas, chain-mapping approaches, quantum Brownian motion master equations, stochastic unravelings, and refined quantum master equations. This diversity, while indicative of the field's relevance, has inadvertently led to a fragmentation that hinders cohesive advances and their effective cross-community application to current problems for complex systems. How are different approaches related to each other? What are their strengths and limitations? Here we give a systematic overview and concise discussion addressing these questions. We make use of a unified framework which very conveniently allows to link different schemes and, this way, may also catalyze further progress. In line with the state of the art, this framework is formulated not in a fully reduced space of the system but in an extended state space which in a minimal fashion includes effective reservoir modes. This in turn offers a comprehensive understanding of existing methods, elucidating their physical interpretations, interconnections, and applicability.