We present an analytical model describing the transition to a strong coupling regime for an ensemble of emitters resonantly coupled to a localized surface plasmon in a metal-dielectric structure. The response of a hybrid system to an external field is determined by two distinct mechanisms involving collective states of emitters interacting with the plasmon mode. The first mechanism is the near-field coupling between the bright collective state and the plasmon mode, which underpins the energy exchange between the system components and gives rise to exciton-induced transparency minimum in scattering spectra in the weak coupling regime and to emergence of polaritonic bands as the system transitions to the strong coupling regime. The second mechanism is the Fano interference between the plasmon dipole moment and the plasmon-induced dipole moment of the bright collective state as the hybrid system interacts with the radiation field. The latter mechanism is greatly facilitated by plasmon-induced coherence in a system with the characteristic size below the diffraction limit as the individual emitters comprising the collective state are driven by the same alternating plasmon near field and, therefore, all oscillate in phase. This cooperative effect leads to scaling of the Fano asymmetry parameter and of the Fano function amplitude with the ensemble size, and therefore, it strongly affects the shape of scattering spectra for large ensembles. Specifically, with increasing emitter numbers, the Fano interference leads to a spectral weight shift toward the lower energy polaritonic band.
We present an analytical model describing the transition to a strong coupling regime for an ensemble of emitters resonantly coupled to a localized surface plasmon in a metal-dielectric structure. The response of a hybrid system to an external field is determined by two distinct mechanisms involving collective states of emitters interacting with the plasmon mode. The first mechanism is the near-field coupling between the bright collective state and the plasmon mode, which underpins the energy exchange between the system components and gives rise to exciton-induced transparency minimum in scattering spectra in the weak coupling regime and to emergence of polaritonic bands as the system transitions to the strong coupling regime. The second mechanism is the Fano interference between the plasmon dipole moment and the plasmon-induced dipole moment of the bright collective state as the hybrid system interacts with the radiation field. The latter mechanism is greatly facilitated by plasmon-induced coherence in a system with the characteristic size below the diffraction limit as the individual emitters comprising the collective state are driven by the same alternating plasmon near field and, therefore, all oscillate in phase. This cooperative effect leads to scaling of the Fano asymmetry parameter and of the Fano function amplitude with the ensemble size, and therefore, it strongly affects the shape of scattering spectra for large ensembles. Specifically, with increasing emitter numbers, the Fano interference leads to a spectral weight shift toward the lower energy polaritonic band.
Quantum coherence controlled by the resonant condition of electromagnetically induced transparency (EIT) has attracted considerable attention for the excitation of surface plasmon polaritons (SPPs) in various metal–dielectric hybrid structures. However, for all coherent fields operating resonantly in the system, the exact extent to which perfect EIT is effective in establishing coupler-free SPP excitation has not yet been well examined. Here, we investigate the excitation of SPPs in an air–metal–atom composite structure incorporating a three-level Λ-type atomic model that operates in the strong ground-state coherence-dephasing regime. Such decoherence limits the establishment of true EIT under the condition of two-photon Raman resonance. It is found that, although the characteristic narrow resonant field enhancement associated with EIT mediated by the resonant fields disappears, significant SPP-assisted field enhancement survives over a broad off-resonant spectral region. This behavior originates from the preservation of the momentum-matching condition together with the fulfillment of the dielectric requirements for surface plasmon resonance (SPR) in the normal-dispersion regime. If the coupling field is tuned to the SPR condition, the detuned two-photon Raman resonance plays a vital role in structuring a doublet in the spectral response of an initially single-peaked broadband SPP excitation. This observation demonstrates that, although true EIT does not occur in the system, an EIT-like plasmonic spectral signature appears through the off-resonant SPP excitation mechanism. All-optical switching can be realized by turning the detuned condition of the coupling field on and off, thereby exhibiting this coherence feature. Furthermore, we show that the present model remains robust in the Doppler-broadened regime, providing a realistic route toward coherence-controlled coupler-free SPP excitation beyond the conventional ideal-EIT framework.
We develop a theory of cooperative emission of light by an ensemble of emitters, such as fluorescing molecules or semiconductor quantum dots, located near a metal nanostructure supporting surface plasmon. The primary mechanism of cooperative emission in such systems is resonant energy transfer between emitters and plasmons rather than the Dicke radiative coupling between emitters. We identify two types of plasmonic coupling between the emitters, (i) plasmon-enhanced radiative coupling and (ii) plasmon-assisted nonradiative energy transfer, the competition between them governing the structure of system eigenstates. Specifically, when emitters are removed by more than several nanometers from the metal surface, the emission is dominated by three superradiant states with the same quantum yield as a single emitter, resulting in a drastic reduction of ensemble radiated energy, while at smaller distances cooperative behavior is destroyed by nonradiative transitions. The crossover between two regimes can be observed in distance dependence of ensemble quantum efficiency. Our numerical calculations incorporating direct and plasmon-assisted interactions between the emitters indicate that they do not destroy the plasmonic Dicke effect.
We develop a theory of cooperative emission of light by an ensemble of emitters, such as fluorescing molecules or semiconductor quantum dots, located near a metal nanostructure supporting surface plasmon. The primary mechanism of cooperative emission in such systems is resonant energy transfer between emitters and plasmons rather than the Dicke radiative coupling between emitters. We identify two types of plasmonic coupling between the emitters, (i) plasmon-enhanced radiative coupling and (ii) plasmon-assisted nonradiative energy transfer, the competition between them governing the structure of system eigenstates. Specifically, when emitters are removed by more than several nm from the metal surface, the emission is dominated by three superradiant states with the same quantum yield as a single emitter, resulting in a drastic reduction of ensemble radiated energy, while at smaller distances cooperative behavior is destroyed by nonradiative transitions. The crossover between two regimes can be observed in distance dependence of ensemble quantum efficiency. Our numerical calculations incorporating direct and plasmon-assisted interactions between the emitters indicate that they do not destroy the plasmonic Dicke effect.
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.
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.
We investigate excitation dynamics in the system of a quantum dipole emitter (QDE) coupled to a located nearby metal nanoparticle (MNP), which exhibits a dipolar localized surface plasmon (LSP) resonance at the frequency of the QDE radiative transition, in the presence of a strong external resonant electromagnetic field. Considering the QDE-field interactions in the regime of strong QDE-field coupling, we show that the feedback provided by the MNP on the QDE (due to the LSP excitation with the field generated by the dipole moment of the QDE transition) influences significantly the coherent process of Rabi oscillations, resulting in the occurrence of additional satellite frequencies in the radiation spectrum scattered by the QDE-MNP configuration. The relative ratio of high harmonics depends strongly on the QDE-MNP separation, an important characteristic feature that can be used for observing this effect and can be exploited, for example, for controlling distances at the nanoscale.