Quantum description and emergence of nonlinearities in strongly coupled single-emitter nanoantenna systems

Rousseaux, Benjamin; Baranov, Denis G.; Käll, Mikael; Shegai, Timur; Johansson, Göran

doi:10.1103/physrevb.98.045435

Cited by 40 publications

(32 citation statements)

References 66 publications

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“…Clearly the output coupling matrix L μη is connected to the radiative part of the QNM decay through the dissipationinduced radiative coupling matrix S rad μη . In contrast, in a phenomenologically dissipative JC output model, one assumes typically uncoupled output radiation, where each mode is coupled out to the surrounding environment independently [49,76]. In the following, we will compare the above formulas using the derived output electric field with the output intensity in a phenomenological dissipative JC modelĨ out = μĨ out μ withĨ out μ ≡ 2ω μ β rad (ω a )γ μ α † μα μ ss ,…”

Section: Output Far Field Intensitymentioning

confidence: 99%

Quantized quasinormal-mode description of nonlinear cavity-QED effects from coupled resonators with a Fano-like resonance

Franke

Richter

Ren

et al. 2020

Phys. Rev. Research

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We employ a recently developed quantization scheme for quasinormal modes (QNMs) to study a nonperturbative open cavity-QED system consisting of a hybrid metal-dielectric resonator coupled to a quantum emitter. This hybrid cavity system allows one to explore the complex coupling between a low-Q (quality factor) resonance and a high-Q resonance, manifesting in a striking Fano resonance, an effect that is not captured by traditional quantization schemes using normal modes or a Jaynes-Cummings (JC)-type model. The QNM quantization approach rigorously includes dissipative coupling between the QNMs and is supplemented with generalized input-output relations for the output electric field operator for multiple modes in the system and correlation functions outside the system. The role of the dissipation-induced mode coupling is explored in the strong coupling regime between the photons and emitter beyond the first rung of the JC dressed-state ladder. Important differences in the quantum master equation and input-output relations between the QNM quantum model and phenomenological dissipative JC models are found. For the hybridized high-Q cavity mode, we show how the dissipation-induced coupling causes a significant reduction in the cavity-emitter coupling rate, and the cavity decay rate, compared to a simpler JC model. In a second step, numerical results for the Fock distributions and system as well as output correlation functions obtained from the quantized QNM model for the hybrid structure are compared with results from a phenomenological approach. We demonstrate explicitly how the quantized QNM model manifests in multiphoton quantum correlations beyond what is predicted by the usual JC models.

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Section: Output Far Field Intensitymentioning

confidence: 99%

Quantized quasinormal-mode description of nonlinear cavity-QED effects from coupled resonators with a Fano-like resonance

Franke

Richter

Ren

et al. 2020

Phys. Rev. Research

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“…Note, that we have phenomenologically included the (free-space or homogeneous background) spontaneous emission (γ) and pure dephasing (γ ) process of the TLS in Eq. (27).…”

Section: B Quantized Quasinormal Mode Theorymentioning

confidence: 99%

“…A further complication is the often ad hoc quantization of the underlying plasmon modes. The most common treatment uses a driven Jaynes-Cumming (JC) model [25][26][27] , which has been used to compare different designs that are assumed to behave like a single mode JC model, then computing quantities like the degree of an-tibunching from a continuous wave (CW) driven system. Thus there is now a pressing need for a more fundamental theory for metallic resonators for SPS applications, and there is a rather urgent need to clarify and quantify the most useful figures of merit for plasmonic SPSs.…”

Section: Introductionmentioning

confidence: 99%

Theory and Limits of On-Demand Single-Photon Sources Using Plasmonic Resonators: A Quantized Quasinormal Mode Approach

et al. 2019

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Quantum emitters coupled to plasmonic resonators are known to allow enhanced broadband Purcell factors, and such systems have been recently suggested as possible candidates for on-demand single photon sources, with fast operation speeds. However, a true single photon source has strict requirements of high efficiency (brightness) and quantum indistinguishability of the emitted photons, which can be quantified through two-photon interference experiments. To help address this problem, we employ and extend a recently developed quantized quasinormal mode approach, which rigorously quantizes arbitrarily lossy open system modes, to compute the key parameters that accurately quantify the figures of merit for plasmon-based single photon sources. We also present a quantized input-output theory to quantify the radiative and nonradiative quantum efficiencies. We exemplify the theory using a nanoplasmonic dimer resonator made up of two gold nanorods, which yields large Purcell factors and good radiative output beta factors. Considering an optically pulsed excitation scheme, we explore the key roles of pulse duration and pure dephasing on the single photon properties, and show that ultrashort pulses (sub-ps) are generally required for such structures, even for low temperature operation. We also quantify the role of the nonradiative beta factor both for single photon and two-photon emission processes. Our general approach can be applied to a wide variety of plasmon systems, including metal-dielectrics, and cavity-waveguide systems, without recourse to phenomenological quantization schemes.

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“…Rabi splitting between single quantum dots and dielectric high-Q microcavities was observed in a number of works but only at cryogenic temperatures [16,17]. Plasmonic nanocavities enable observation of strong coupling with quantum dots and organic chromophores at room temperatures [18][19][20][21][22], but most of such structures are at the border between the weak and the strong coupling regimes due to limited coupling strength [23].…”

Section: Introductionmentioning

confidence: 99%

“…Our results could potentially help in understanding the microscopic behavior of experimental observations of QE-plasmon systems such as those shown in Refs. [19,20], where a single emitter strong coupling was demonstrated but modeling the system with a single mode for the plasmonic response yields unrealistic values for the dipole moments of the QE [23].…”

Section: Introductionmentioning

confidence: 99%

Strong coupling as an interplay of quantum emitter hybridization with plasmonic dark and bright modes

Rousseaux

Baranov

Antosiewicz

et al. 2020

Phys. Rev. Research

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Strong coupling between a single quantum emitter and an electromagnetic mode is one of the key effects in quantum optics. In the cavity QED approach to plasmonics, strongly coupled systems are usually understood as single-transition emitters resonantly coupled to a single radiative plasmonic mode. However, plasmonic cavities also support nonradiative (or "dark") modes, which offer much higher coupling strengths. On the other hand, realistic quantum emitters often support multiple electronic transitions of various symmetries, which could overlap with higher order plasmonic transitions-in the blue or ultraviolet part of the spectrum. Here, we show that despite very large detuning between a bright mode and an excitonic transition, their strong coupling can be ensured by leveraging higher energy dark modes of the optical cavity. Specifically, when a dark mode interacts strongly with an excitonic transition, the lower polariton of the hybridized spectrum can be pushed to energies of the bright mode. The resulting interaction of the lower dark-mode-exciton polariton and bright mode yields significant vacuum Rabi splitting, which hinges on the existence of the dark mode. We develop a simple model illustrating the modification of the system response in the "dark" strong coupling regime and demonstrate single photon nonlinearity. These results may find important implications in the emerging field of room-temperature quantum plasmonics.

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Quantum description and emergence of nonlinearities in strongly coupled single-emitter nanoantenna systems

Cited by 40 publications

References 66 publications

Quantized quasinormal-mode description of nonlinear cavity-QED effects from coupled resonators with a Fano-like resonance

Quantized quasinormal-mode description of nonlinear cavity-QED effects from coupled resonators with a Fano-like resonance

Theory and Limits of On-Demand Single-Photon Sources Using Plasmonic Resonators: A Quantized Quasinormal Mode Approach

Strong coupling as an interplay of quantum emitter hybridization with plasmonic dark and bright modes

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