Interplay between Static and Dynamic Disorder: Contrasting Effects on Dark State Population inside a Cavity

Abstract

Strong light-matter interactions between molecules and quantized electromagnetic fields inside an optical cavity open up novel possibilities, though inevitably influenced by disorder, an inherent attribute of realistic molecular systems. Here, we explore the steady-state optical response of molecular emitters within a lossy cavity, with a focus on the combined effects of static and dynamic disorder, as frequently observed in solution-phase experiments. By analyzing the transmission spectra, molecular energy change, and dark state population, we uncover the contrasting effects of static and dynamic disorder on the dark state population and its interplay with polariton states. We find that the Rabi splitting exhibits an inversion with increasing disorder strength where the maximum splitting is determined by the interplay of static and dynamic disorder. Furthermore, we identify a dark state-induced polariton linewidth narrowing, revealing a mechanism distinct from motional narrowing induced by frequency fluctuations. These mechanistic insights highlight the critical role of dark states, establishing a foundation for future developments in the fields of polariton chemistry and strong coupling spectroscopy.

References in corpus (13)

• Catalysis by Dark States in Vibropolaritonic Chemistry
• Polariton Localization and Dispersion Properties of Disordered Quantum Emitters in Multimode Microcavities
• Microscopic Theory of Multimode Polariton Dispersion in Multilayered Materials
• Effects of disorder on polaritonic and dark states in a cavity using the disordered Tavis-Cummings model
• Exploring the impact of vibrational cavity coupling strength on ultrafast CN + $c$-C${}_6$H${}_{12}$ reaction dynamics
• Disorder-enhanced transport in a chain of lossy dipoles strongly coupled to cavity photons
• Controlling the Manifold of Polariton States Through Molecular Disorder
• Interplay Between Disorder and Collective Coherent Response: Superradiance and Spectral Motional Narrowing in the Time Domain
• A versatile platform for gas-phase molecular polaritonics
• Probing anomalous relaxation by coherent multidimensional optical spectroscopy
• Efficient parallel strategy for molecular plasmonics -- a numerical tool for integrating Maxwell-Schrodinger equations in three dimensions
• Unraveling Abnormal Collective Effects via the Non-Monotonic Number Dependence of Electron Transfer in Confined Electromagnetic Fields
• Anomalous Giant Superradiance in Molecular Aggregates Coupled to Polaritons

Cited by in corpus (4)

• Mean-field Mixed Quantum-Classical Approach for Many-Body Quantum Dynamics of Exciton-Polaritons
• Dissecting Exciton-Polariton Transport in Organic Molecular Crystals: Emerging Conductivity Assisted by Intermolecular Vibrational Coupling
• Mechanistic principles of exciton-polariton relaxation
• Elucidating the Synergetic Interplay between Average Intermolecular Coupling and Coupling Disorder in Short-Time Exciton Transfer