Interplay Between Disorder and Collective Coherent Response: Superradiance and Spectral Motional Narrowing in the Time Domain

Abstract

The interplay between static and dynamic disorder and collective optical response in molecular ensembles is an important characteristic of nanoplasmonic and nanophotonic molecular systems. Here we investigate the cooperative superradiant response of a molecular ensemble of quantum emitters under the influence of environmental disorder, including inhomogeneous broadening (as induced by static random distribution of the molecular transition frequencies) and motional narrowing (as induced by stochastic modulation of these excitation energies). The effect of inhomogeneous broadening is to destroy the coherence of the collective molecular excitation and suppress superradiant emission. However, fast stochastic modulation of the molecular excitation energy can effectively restore the coherence of the quantum emitters and lead to a recovery of superradiant emission, which is an unexpected manifestation of motional narrowing. For a light scattering process as induced by an off-resonant incident pulse, stochastic modulation leads to inelastic fluorescence emission at the average excitation energy at long times and suggests that dynamic disorder effects can actually lead to collective excitation of the molecular ensemble.

References in corpus (31)

• Superfluorescence from Lead Halide Perovskite Quantum Dot Superlattices
• Superradiance for atoms trapped along a photonic crystal waveguide
• Exponential improvement in photon storage fidelities using subradiance and "selective radiance" in atomic arrays
• Subradiance in a Large Cloud of Cold Atoms
• Cavity-induced modifications of molecular structure in the strong coupling regime
• A subradiant optical mirror formed by a single structured atomic layer
• Unconventional motional narrowing in the optical spectrum of a semiconductor quantum dot
• Collective atomic scattering and motional effects in a dense coherent medium
• Controlled Dicke Subradiance from a Large Cloud of Two-Level Systems
• Theory of Subradiant States of a One-Dimensional Two-Level Atom Chain
• Observation of room-temperature spontaneous superradiance from single diamond nanocrystals
• Generation and controllable switching of superradiant and subradiant states in a 10-qubit superconducting circuit
• Super-Radiant Dynamics, Doorways, and Resonances in Nuclei and Other Open Mesoscopic Systems
• Unusual Dynamical Properties of Disordered Polaritons in Micocavities
• A Class of Fast Methods for Processing Irregularly Sampled or Otherwise Inhomogeneous One-Dimensional Data
• Cooperative Robustness to Static Disorder: Superradiance and localization in a nanoscale ring to model natural light-harvesting systems
• Subradiant Dimer Excitations of Emitter Chains Coupled to a 1D Waveguide
• Optical waveguiding by atomic entanglement in multilevel atom arrays
• Non-Hermitian Hamiltonian approach to quantum transport in disordered networks with sinks: validity and effectiveness
• Interplay of superradiance and disorder in the Anderson Model
• Cooperative robustness to dephasing: single-exciton Superradiance in a nanoscale ring to model natural light-harvesting systems
• Subradiant hybrid states in the open 3D Anderson-Dicke model
• Robustness of Dicke subradiance against thermal decoherence
• Interfering Doorway States and Giant Resonances. I: Resonance Spectrum and Multipole Strengths
• Organic Molecular Dynamics and Charge-carrier Lifetime in Lead Iodide Perovskite MAPbI${}_3$
• Collective Dissipative Molecule Formation in a Cavity
• Doorway states in nuclear reactions as a manifestation of the "super-radiant" mechanism
• Exact $k$-body representation of the Jaynes-Cummings interaction in the dressed basis: Insight into many-body phenomena with light
• Energy transfer and interference by collective electromagnetic coupling
• Electromagnetically Induced Transparency with Superradiant and Subradiant states
• Disordered ensembles of strongly coupled single-molecule plasmonic picocavities as nonlinear optical metamaterials

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• Collective Polaritonic Effects on Chemical Dynamics Suppressed by Disorder
• Nonlinear semiclassical spectroscopy of ultrafast molecular polariton dynamics
• Comparing semiclassical mean-field and 1-exciton approximations in evaluating optical response under strong light-matter coupling conditions
• Anomalous Giant Superradiance in Molecular Aggregates Coupled to Polaritons
• Modifying cooperative decay via disorder in atom arrays
• Interplay between Static and Dynamic Disorder: Contrasting Effects on Dark State Population inside a Cavity
• Theory of Molecular Emission Power Spectra. III. Non-Hermitian Interactions in Multichromophoric Systems Coupled with Polaritons