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The Journal of Physical Chemistry C

Exploring Superradiance Effects of Molecular Emitters Coupled with Cavity Photons and Plasmon Polaritons: A Perspective from Macroscopic Quantum Electrodynamics

Siwei Wang, Liang‐Yan Hsu

Published Jun 27, 2023• 9 citations
Publisher

Abstract

In this study, we present the superradiance effects of N identical molecular emitters inside Fabry–Pérot (FP) cavity systems in the framework of macroscopic quantum electrodynamics. The proposed theory can estimate the enhancement of spontaneous emission rates, including the effects of cavity geometry and material dielectric properties. Moreover, our study connects the multichromophoric excitation energy transfer theory and the Tavis–Cummings model via identical cooperative decay rates and dipole–dipole shifts. For molecules resonant with the cavity photon mode, we find that the enhancement is not exactly proportional to N even in a perfect FP cavity due to the effects of electrostatic dipole–dipole interactions. Moreover, in a silver FP cavity, our simulation shows that the enhancement saturates for a large N, indicating that the cavity photon mode can lead to only the collective emission of a limited number of molecules. For molecules in the proximity of the silver mirror, we demonstrate that under specific conditions, the subradiance of molecular emitters can occur through surface plasmon polaritons. Our study not only provides new insights into the mechanism of superradiance effects but also demonstrates that collective effects such as superradiance and subradiance can be controlled by manipulating the dielectric environments.

DOI
10.1021/acs.jpcc.3c02760

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In this study, we present the superradiance effects of N identical molecular emitters inside Fabry–Pérot (FP) cavity systems in the framework of macroscopic quantum electrodynamics. The proposed theory can estimate the enhancement of spontaneous emission rates, including the effects of cavity geometry and material dielectric properties. Moreover, our study connects the multichromophoric excitation energy transfer theory and the Tavis–Cummings model via identical cooperative decay rates and dipole–dipole shifts. For molecules resonant with the cavity photon mode, we find that the enhancement is not exactly proportional to N even in a perfect FP cavity due to the effects of electrostatic dipole–dipole interactions. Moreover, in a silver FP cavity, our simulation shows that the enhancement saturates for a large N, indicating that the cavity photon mode can lead to only the collective emission of a limited number of molecules. For molecules in the proximity of the silver mirror, we demonstrate that under specific conditions, the subradiance of molecular emitters can occur through surface plasmon polaritons. Our study not only provides new insights into the mechanism of superradiance effects but also demonstrates that collective effects such as superradiance and subradiance can be controlled by manipulating the dielectric environments.
We study a molecular emitter above a silver surface in the framework of macroscopic quantum electrodynamics and explore the population dynamics including non-Markovian effects. The theory we present is general for molecular fluorescence in the presence of dielectrics with any space-dependent, frequency-dependent, or complex dielectric functions. Furthermore, the proposed theory allows us to calculate the memory kernel of polaritons using computational electrodynamics packages. In the limit of a high vibration frequency, the different strengths of exciton-polariton couplings lead to distinct characteristics in the population dynamics, e.g., Franck-Condon-Rabi oscillation. (The frequency of Rabi oscillation is dependent on the Franck-Condon factor.) Additionally, in a specific condition, we derive a parameter-free formula that can be used to estimate the exciton-polariton coupling between a molecular emitter and a nanocavity, and the coupling estimated by our theory is in good agreement with the reported experimental results [Chikkaraddy et al., Nature 535, 127-130 (2016)].
We demonstrate a plasmonic route to superradiance and subradiance effects over distances comparable to the operating wavelength. Superradiant and subradiant modes are excited by a collection of two-level quantum emitters inside plasmonic nanochannels. These channels can provide an effective epsilon-near-zero operation in their cut-off frequency and Fabry-P\'erot resonances at higher frequencies. The related plasmonic resonant modes are found to efficiently enhance the constructive (superradiance) or destructive (subradiance) interference between different quantum emitters located inside the nanochannels. By increasing the number of emitters located in the elongated plasmonic channel, the superradiance effect is enhanced at the epsilon-near-zero operation, leading to a strong increase in the collective spontaneous emission rate. In addition, the separation distance between neighboring emitters and their emission wavelengths can be changed to dynamically control the collective emission properties of the plasmonic system. It is envisioned that the dynamic modification between quantum superradiant and subradiant modes will find applications in quantum communication and computing systems.
Surface plasmon polaritons are charge density waves of electrons in a metal, which are coupled to an electromagnetic field at a metal-dielectric interface. The electro- magnetic field associated with surface plasmons is confined, resulting in increased field intensities near the interface. Optical emitters placed near a metal film interact strongly with the surface plasmon modes present, not only modifying the radiation rates, but also the radiation profile. These emitters may be used to store and process information, and understanding their behaviour in the presence of a lossy metal film is important in determining the advantages and limitations of using surface plasmons. In this thesis, we wish to understand how we can optically control atoms by exploring two physical phenomena: first, the influence of surface plasmons on collective effects in an ensemble of emitters. Secondly, the single photon excitation of an emitter near a metal film. In the first case, we analyze the collective radiative behaviour of multiple classical emitters near a metal film that radiatively couple to the far-field through surface plasmon modes. We demonstrate that the contributions of dipolar image charges within the metal film significantly affect the cooperative emission of nearby sources, generating sub- and super-radiant emission that can be controlled with a suitably detuned external driving field. In the second case, we determine the excitation probability of an atom near a metal film by a single photon pulse that is time reversed. Using a quantum electro- dynamic description of absorbing dielectrics, we show that non-radiative decay will limit the excitation probability to about half of the maximum that could be achieved in the absence of losses.
We demonstrate a plasmonic route to control the collective spontaneous emission of two-level quantum emitters. Superradiance and subradiance effects are observed over distances comparable to the operating wavelength inside plasmonic nanochannels. These plasmonic waveguides can provide an effective epsilon-near-zero operation in their cut-off frequency and Fabry-Pérot resonances at higher frequencies. The related plasmonic resonant modes are found to efficiently enhance the constructive (superradiance) or destructive (subradiance) interference between different quantum emitters located inside the waveguides. By increasing the number of emitters located in the elongated plasmonic channel, the superradiance effect is enhanced at the epsilon-near-zero operation, leading to a strong coherent increase in the collective spontaneous emission rate. In addition, the separation distance between neighboring emitters and their emission wavelengths can be changed to dynamically control the collective emission properties of the plasmonic system. It is envisioned that the dynamic modification between quantum superradiant and subradiant modes will find applications in quantum entanglement of qubits, low-threshold nanolasers and efficient sensors.
Spontaneous emission from ensembles of quantum emitters (QEs) such as atoms, molecules or semiconductor quantum dots can be greatly enhanced by cooperative effects arising from electromagnetic correlations. We describe a cooperative mechanism for emission of light by an ensemble of QEs based upon cooperative energy transfer from QEs to localized surface plasmons in metal-dielectric structures followed by plasmon radiation at a rate that scales with the ensemble size. For large QE ensembles saturating the plasmon mode volume, we derive universal, i.e. independent of local field distribution, expression for cooperative Purcell factor that can by far exceed the field enhancement limits for individual QE in a hot spot. We also derive radiated power spectrum that retains the plasmon resonance lineshape and, in contrast to common cooperative mechanisms, is insensitive to natural variations of QEs' emission frequencies.
Cavity-embedded quantum emitters show strong modifications of free space radiation properties such as an enhanced decay known as the Purcell effect. The central parameter is the cooperativity CCC, the ratio of the square of the coherent cavity coupling strength over the product of cavity and emitter decay rates. For a single emitter, CCC is independent of the transition dipole moment and dictated by geometric cavity properties such as finesse and mode waist. In a recent work [Phys. Rev. Lett. 119, 093601 (2017)], we have shown that collective excitations in ensembles of dipole-dipole coupled quantum emitters show a disentanglement between the coherent coupling to the cavity mode and spontaneous free space decay. This leads to a strong enhancement of the cavity cooperativity around certain collective subradiant antiresonances. Here, we present a quantum Langevin equations approach aimed at providing results beyond the classical coupled dipoles model. We show that the subradiantly enhanced cooperativity imprints its effects onto the cavity output field quantum correlations while also strongly increasing the cavity-emitter system's collective Kerr nonlinear effect.