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International Congress on Artificial Materials for Novel Wave Phenomena (Metamaterials)

Photonic Modelling of Two-Photon Purcell Effect Near Plasmonic Nanostructures

S. Smeets, Björn Maes, Gilles Rosolen

Published Sep 11, 2023• 0 citations
Publisher

Abstract

We present a novel photonic model that enables an efficient computation of the two-photon Purcell effect of a quantum emitter in the vicinity of an arbitrary photonic structure. Our framework is relevant for the plasmonic nanocavities used to enhance higher-order light-matter interactions, as it goes beyond the dipolar approximation. The computation of Purcell factors through classical electromagnetic simulations determines the influence of the environment without tedious analytic calculations. We demonstrate that placing a hydrogen-like emitter close to a silver nanodisk enhances the transition rate by 5 and 11 orders of magnitude via electric dipole and quadrupole two-photon transitions, respectively. This process has exciting implications for future research, including the potential for efficient entangled two-photon sources.

DOI
10.1109/metamaterials58257.2023.10289352

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We present a novel photonic model that enables an efficient computation of the two-photon Purcell effect of a quantum emitter in the vicinity of an arbitrary photonic structure. Our framework is relevant for the plasmonic nanocavities used to enhance higher-order light-matter interactions, as it goes beyond the dipolar approximation. The computation of Purcell factors through classical electromagnetic simulations determines the influence of the environment without tedious analytic calculations. We demonstrate that placing a hydrogen-like emitter close to a silver nanodisk enhances the transition rate by 5 and 11 orders of magnitude via electric dipole and quadrupole two-photon transitions, respectively. This process has exciting implications for future research, including the potential for efficient entangled two-photon sources.
We develop a framework that computes two-photon spontaneous emission (TPSE) spectra of a quantum emitter near an arbitrarily shaped nanostructure. The model considers the interaction up to the electric quadrupolar order, which is relevant for nanophotonic structures sustaining strongly confined fields that are used to enhance and to tailor spontaneous emission processes. Moreover, we consider interference effects between multipolar two-photon emission channels, for the first time to our knowledge. First, we show for a s → s transition of a hydrogen atom placed under a silver plasmonic nanodisk a substantial enhancement in the photon-pair emission rates by 5 and 11 orders of magnitude for the two-electric dipole (2ED) and two-electric quadrupole (2EQ) transitions, respectively. Then for the same emitter under a plasmonic graphene nanotriangle, we demonstrate a breakdown of the electric dipole approximation in the TPSE process where the interference between the 2ED and 2EQ transitions is important, as it increases the total rate by 63 %. Third, we explore platforms where entangled photons of different energy are emitted in the far-field in different directions. In the end, our framework is a complete tool to design emitters and nanostructures for the TPSE process, leading to a rich assortment of functional nanoantennas.
The rate of spontaneous emission is known to depend on the environment of a emitter, and the enhancement of one-photon emission in a resonant cavity is known as the Purcell effect. Here we develop a theory of spontaneous two-photon emission for a general electromagnetic environment including inhomogeneous dispersive and absorptive media. This theory is used to evaluate the two-photon Purcell enhancement in the vicinity of metallic nanoparticles and demonstrates that the surface-plasmon resonances supported by these particles can increase the emission rate by more than two orders of magnitude. The control over two-photon Purcell enhancement given by tailored nanostructured environments could provide an emitter with any desired spectral response and may serve as an ultimate route for designing light sources with novel properties.
We summarize our studies of the plasmonic enhancements of the spontaneous two-photon emission. In particular, we draw attention to the rigorous investigation of quantum framework for the multi-photon spontaneous decay rates in an environment with arbitrary structure of electromagnetic modes. We demonstrate that nanostructured environment can be used for tailoring the basic characteristics of the two-photon emission such as spectrum, lifetime, and entanglement. Moreover, careful engineering of the two-photon Purcell enhancement may provide any desired spectral response and may serve as an ultimate route for designing light sources with novel properties.
Summary form only given. In the pioneering work of Purcell, the possibility to control spontaneous emission lifetimes of quantum emitters by tailoring their electromagnetic surroundings was widely investigated and verified in various types of cavities or band-gap environments. This includes semiconductor microstructures, photonic crystals, and plasmonic nanoparticles. Due to the extraordinary ability of plasmonic nanostructures to confine light into subwavelength spatial domains, steps beyond the paradigmatic electric dipole approximation in the theoretical description of this process may be necessary. In this contribution, we focus on the case of multiple in general nonidentical two-level emitters, sharing the same electromagnetic surroundings, whose local density of states could be tailored by a neighbouring nanostructure. In this case, the surroundings may serve as a long-distance emitter-emitter interaction carrier, or it may trigger collective emission processes, in analogy to Dicke superradiance. We describe these phenomena taking into account the electric dipole, magnetic dipole and electric quadrupole components of light-matter interaction Hamiltonian.
Several methods have been developed to calculate the spontaneous emission rate for extended emitters in the vicinity of a nanophotonic structure.While taking the emitter's spatial extension, these methods have taken approximations regarding the full interaction, either by coupling to one single plasmonic mode or adding higher order rates individually thus neglecting interference terms.Here we apply a new framework [1] to extended emitters, by which, all these interactions can be considered, and we show both under, and over-estimation of the Purcell Factor when using a point-dipole.