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arXiv:2101.03571 · Applied Physics Letters

Spontaneous emission dynamics of Eu3+ ions coupled to hyperbolic metamaterials

Gabriel I. López-Morales, Mingxing Li, Ravindra K. Yadav, Harshavardhan Reddy Kalluru, Jaydeep K. Basu, Carlos A. Meriles, Vinod M. Menon

Published Jan 4, 2021• 8 citations
arXivHTMLPDF

Abstract

Sub-wavelength nanostructured systems with tunable electromagnetic properties, such as hyperbolic metamaterials (HMMs), provide a useful platform to tailor spontaneous emission processes. Here, we investigate a system comprising Eu3+(NO3)3·6H2O nanocrystals on an HMM structure featuring a hexagonal array of Ag nanowires in a porous Al2O3 matrix. The HMM-coupled Eu3+ ions exhibit up to a 2.4 fold increase in their decay rate, accompanied by an enhancement of the emission rate of the 5D0 → 7F2 transition. Using finite-difference time-domain modeling, we corroborate these observations with the increase in the photonic density of states seen by the Eu3+ ions in the proximity of the HMM. Our results indicate that HMMs can serve as a valuable tool to control the emission from weak transitions and, hence, hint at a route toward more practical applications of rare-earth ions in nanoscale optoelectronics and quantum devices.

DOI
10.1063/5.0032529

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Sub-wavelength nanostructured systems with tunable electromagnetic properties, such as hyperbolic metamaterials (HMMs), provide a useful platform to tailor spontaneous emission processes. Here, we investigate a system comprising Eu3+(NO3)3·6H2O nanocrystals on an HMM structure featuring a hexagonal array of Ag nanowires in a porous Al2O3 matrix. The HMM-coupled Eu3+ ions exhibit up to a 2.4 fold increase in their decay rate, accompanied by an enhancement of the emission rate of the 5D0 → 7F2 transition. Using finite-difference time-domain modeling, we corroborate these observations with the increase in the photonic density of states seen by the Eu3+ ions in the proximity of the HMM. Our results indicate that HMMs can serve as a valuable tool to control the emission from weak transitions and, hence, hint at a route toward more practical applications of rare-earth ions in nanoscale optoelectronics and quantum devices.
Within the frame of quantum optics we analyze the properties of spontaneous emission of two-level atom in media with indefinite permittivity tensor where the geometry of the dispersion relation is characterized by an ellipsoid or a hyperboloid(hyperbolic medium). The decay rate is explicitly given with the orientation of the dipole transition matrix element taken into account. It indicates that for the ellipsoid case the intensity of the photons coupled into different modes can be tuned by changing the direction of the matrix element and for the hyperboloid case it is found that spontaneous emission in hyperbolic medium can be dramatically enhanced compared to the dielectric background. Moreover, spontaneous emission exhibit the strong directivity and get the maximum in the asymptote direction.
Single-photon and correlated two-photon sources are important elements for optical information systems. Nonlinear downconversion light sources are robust and stable emitters of single photons and entangled photon pairs. However, the rate of downconverted light emission, dictated by the properties of low-symmetry nonlinear crystals, is typically very small, leading to significant constrains in device design and integration. In this paper, we show that the principles for spontaneous emission control (i.e. Purcell effect) of isolated emitters in nanoscale structures, such as metamaterials, can be generalized to describe the enhancement of nonlinear light generation processes such as parametric down conversion. We develop a novel theoretical framework for quantum nonlinear emission in a general anisotropic, dispersive and lossy media. We further find that spontaneous parametric downconversion in media with hyperbolic dispersion is broadband and phase-mismatch-free. We predict a 1000-fold enhancement of the downconverted emission rate with up to 105 photon pairs per second in experimentally realistic nanostructures. Our theoretical formalism and approach to Purcell enhancement of nonlinear optical processes, provides a framework for description of quantum nonlinear optical phenomena in complex nanophotonic structures.
The interaction of single quantum emitters with an optical cavity enables the realization of efficient spin-photon interfaces, an essential resource for quantum networks. The dynamical control of the spontaneous emission rate of quantum emitters in cavities has important implications in quantum technologies, e.g., for shaping the emitted photons' waveform or for driving coherently the optical transition while preventing photon emission. Here we demonstrate the dynamical control of the Purcell enhanced emission of a small ensemble of erbium ions doped into a nanoparticle. By embedding the nanoparticles into a fully tunable high finesse fiber based optical microcavity, we demonstrate a median Purcell factor of 15 for the ensemble of ions. We also show that we can dynamically control the Purcell enhanced emission by tuning the cavity on and out of resonance, by controlling its length with sub-nanometer precision on a time scale more than two orders of magnitude faster than the natural lifetime of the erbium ions. This capability opens prospects for the realization of efficient nanoscale quantum interfaces between solid-state spins and single telecom photons with controllable waveform, for non-destructive detection of photonic qubits, and for the realization of quantum gates between rare-earth ion qubits coupled to an optical cavity.
We report on the coupling of the emission from a single europium-doped nanocrystal to a fiber-based microcavity under cryogenic conditions. As a first step, we study the properties of nanocrystals that are relevant for cavity experiments and show that embedding them in a dielectric thin film can significantly reduce scattering loss and increase the light–matter coupling strength for dopant ions. The latter is supported by the observation of a fluorescence lifetime reduction, which is explained by an increased local field strength. We then couple an isolated nanocrystal to an optical microcavity, determine its size and ion number, and perform cavity-enhanced spectroscopy by resonantly coupling a cavity mode to a selected transition. We measure the inhomogeneous linewidth of the coherent transition and find a value that agrees with the linewidth in bulk crystals, evidencing a high crystal quality. We detect the fluorescence from an ensemble of few ions in the regime of power broadening and observe an increased fluorescence rate consistent with Purcell enhancement. The results represent an important step towards the efficient readout of single rare earth ions with excellent optical and spin coherence properties, which is promising for applications in quantum communication and distributed quantum computation.
Photonic crystals based on silica colloidal crystals (artificial opals) exhibit pronounced stopbands for electromagnetic wave propagation and the corresponding modification of the photon density of states in the visible range. These spectrally selective features can be enhanced by impregnating opals with higher refractive materials like, e.g., polymers. Doping of these structures with dye molecules, semiconductor nanoparticles (quantum dots), and rare-earth ions provides a possibility to examine the challenging theoretical predictions of the inhibited spontaneous emission in photonic bandgap (PBG) materials. First experiments are discussed in which pronounced modification of spontaneous emission spectra and noticeable changes in decay kinetics were observed.
Abstract The interaction of single quantum emitters with an optical cavity enables the realization of efficient spin-photon interfaces, an essential resource for quantum networks. The dynamical control of the spontaneous emission rate of quantum emitters in cavities has important implications in quantum technologies, e.g., for shaping the emitted photons’ waveform or for driving coherently the optical transition while preventing photon emission. Here we demonstrate the dynamical control of the Purcell enhanced emission of a small ensemble of erbium ions doped into a nanoparticle. By embedding the nanoparticles into a fully tunable high finesse fiber based optical microcavity, we demonstrate a median Purcell factor of 15 for the ensemble of ions. We also show that we can dynamically control the Purcell enhanced emission by tuning the cavity on and out of resonance, by controlling its length with sub-nanometer precision on a time scale more than two orders of magnitude faster than the natural lifetime of the erbium ions. This capability opens prospects for the realization of efficient nanoscale quantum interfaces between solid-state spins and single telecom photons with controllable waveform, for non-destructive detection of photonic qubits, and for the realization of quantum gates between rare-earth ion qubits coupled to an optical cavity.