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Localized-surface plasmon resonance is of importance in both fundamental and applied physics for the subwavelength confinement of optical field, but realization of quantum coherent processes is confronted with challenges due to strong dissipation. Here we propose to engineer the electromagnetic environment of metallic nanoparticles (MNPs) using optical microcavities. An analytical quantum model is built to describe the MNP-microcavity interaction, revealing the significantly enhanced dipolar radiation and consequentially reduced Ohmic dissipation of the plasmonic modes. As a result, when interacting with a quantum emitter, the microcavity-engineered MNP enhances the quantum yield over 40 folds and the radiative power over one order of magnitude. Moreover, the system can enter the strong coupling regime of cavity quantum electrodynamics, providing a promising platform for the study of plasmonic quantum electrodynamics, quantum information processing, precise sensing and spectroscopy.
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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 non-radiative (or dark) modes, which offer much higher coupling strengths. On the other hand, realistic quantum emitters often support multiple electronic transitions of various symmetry, which could overlap with higher order plasmonic transitions -- in the blue or ultraviolet part of the spectrum. Here, we show that vacuum Rabi splitting with a single emitter can be achieved by leveraging dark modes of a plasmonic nanocavity. Specifically, we show that a significantly detuned electronic transition can be hybridized with a dark plasmon pseudomode, resulting in the vacuum Rabi splitting of the bright dipolar plasmon mode. We develop a simple model illustrating the modification of the system response in the dark strong coupling regime and demonstrate single photon non-linearity. These results may find important implications in the emerging field of room temperature quantum plasmonics.
Coupling $N$ identical emitters to the same field mode is well-established method to enhance light matter interaction. However, the resulting $sqrt{N}$ boost of the coupling strength comes at the cost of a linearized (effectively semi-classical) dynamics. Here, we instead demonstrate a new approach for enhancing the coupling constant of a textit{single} quantum emitter, while retaining the nonlinear character of the light-matter interaction. We consider a single quantum emitter with $N$ nearly degenerate transitions that are collectively coupled to the same field mode. We show that in such conditions an effective Jaynes-Cummings model emerges, with a boosted coupling constant of order $sqrt{N}$. The validity and consequences of our general conclusions are analytically demonstrated for the instructive case $N=2$. We further observe that our system can closely match the spectral line shapes and photon autocorrelation functions typical of Jaynes-Cummings physics, hence proving that quantum optical nonlinearities are retained. Our findings match up very well with recent broadband plasmonic nanoresonator strong-coupling experiments and will therefore facilitate the control and detection of single-photon nonlinearities at ambient conditions.
We present an overview of the framework of macroscopic quantum electrodynamics from a quantum nanophotonics perspective. Particularly, we focus our attention on three aspects of the theory which are crucial for the description of quantum optical phenomena in nanophotonic structures. First, we review the light-matter interaction Hamiltonian itself, with special emphasis on its gauge independence and the minimal and multipolar coupling schemes. Second, we discuss the treatment of the external pumping of quantum-optical systems by classical electromagnetic fields. Third, we introduce an exact, complete and minimal basis for the field quantization in multi-emitter configurations, which is based on the so-called emitter-centered modes. Finally, we illustrate this quantization approach in a particular hybrid metallodielectric geometry: two quantum emitters placed in the vicinity of a dimer of Ag nanospheres embedded in a SiN microdisk.
Strong and ultra-strong light-matter coupling are remarkable phenomena of quantum electrodynamics occurring when the interaction between a matter excitation and the electromagnetic field cannot be described by usual perturbation theory. This is generally achieved by coupling an excitation with large oscillator strength to the confined electromagnetic mode of an optical microcavity. In this work we demonstrate that strong/ultra-strong coupling can also take place in the absence of optical confinement. We have studied the non-perturbative spontaneous emission of collective excitations in a dense two-dimensional electron gas that superradiantly decays into free space. By using a quantum model based on the input-output formalism, we have derived the linear optical properties of the coupled system and demonstrated that its eigenstates are mixed light-matter particles, like in any system displaying strong or ultra-strong light-matter interaction. Moreover, we have shown that in the ultra-strong coupling regime, i.e. when the radiative broadening is comparable to the matter excitation energy, the commonly used rotating-wave and Markov approximations yield unphysical results. Finally, the input-output formalism has allowed us to prove that Kirchhoffs law, describing thermal emission properties, applies to our system in all the light-matter coupling regimes considered in this work.
Hybrid molecular-plasmonic nanostructures have demonstrated their potential for surface enhanced spectroscopies, sensing or quantum control at the nanoscale. In this work, we investigate the strong coupling regime and explicitly describe the hybridization between the localized plasmons of a metal nanoparticle and the excited state of a quantum emitter, offering a simple and precise understanding of the energy exchange in full analogy with cavity quantum electrodynamics treatment and dressed atom picture. Both near field emission and far field radiation are discussed, revealing the richness of such optical nanosources.
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