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Conference on Lasers and Electro-Optics

Enhancement of Magnetic Dipole Transitions in Lanthanide Ions for Optical Metamaterials

Sinan Karaveli, Alexandra Witthoft, Rashid Zia

Published Jan 1, 2009• 0 citations
Publisher

Abstract

We present experimental evidence of optically enhanced magnetic dipole transitions from trivalent Europium ions. Spectra and lifetime data are used to highlight direct and indirect enhancement pathways, and implications for optical metamaterials are discussed.
DOI
10.1364/iqec.2009.itua4

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Given growing interest in optical-frequency magnetic dipole transitions, we use intermediate coupling calculations to identify strong magnetic dipole emission lines that are well suited for experimental study. The energy levels for all trivalent lanthanide ions in the 4fn4{f}^{\text{n}}4fn configuration are calculated using a detailed free ion Hamiltonian, including electrostatic and spin-orbit terms as well as two-body, three-body, spin-spin, spin-other-orbit, and electrostatically correlated spin-orbit interactions. These free ion energy levels and eigenstates are then used to calculate the oscillator strengths for all ground-state magnetic dipole absorption lines and the spontaneous emission rates for all magnetic dipole emission lines including transitions between excited states. A large number of strong magnetic dipole transitions are predicted throughout the visible and near-infrared spectrum, including many at longer wavelengths that would be ideal for experimental investigation of magnetic light-matter interactions with optical metamaterials and plasmonic antennas.
We demonstrate that magnetic dipole transitions provide an additional degree of freedom for engineering emission spectra. Without the need for a high-quality optical cavity, we show how a simple gold mirror can strongly tune the emission of trivalent europium. We exploit the differing field symmetries of electric and magnetic dipoles to selectively direct the majority of emission through each of three major transitions (centered at 590, 620, and 700 nm), and present a model that accurately predicts this tuning from the local electric and magnetic density of optical states.
Tremendous advances in the study of magnetic light-matter interactions have recently been achieved using man-made nanostructures that exhibit and exploit an optical magnetic response. However, naturally occurring emitters can also exhibit magnetic resonances in the form of optical-frequency magnetic-dipole transitions. Here we quantify the magnetic nature of light emission using energy- and momentum-resolved spectroscopy, and leverage a pair of spectrally close electric- and magnetic-dipole transitions in trivalent europium to probe vacuum fluctuations in the electric and magnetic fields at the nanometre scale. These results reveal a new tool for nano-optics: an atomic-size quantum emitter that interacts with the magnetic component of light. Light-matter interactions are generally dominated by electric fields and electric-dipole transitions. This study, however, quantifies magnetic contributions to light emission and so exploits the strong natural magnetic-dipole transitions in lanthanide ions to measure optical-frequency magnetic fields.
A thorough analysis of the emission via the magnetic dipole (MD) transition, called magnetic light below, of trivalent rare-earth ions in or near dielectric homogeneous spheres has been performed. In the search for enhancement of fluorescence from magnetic light, one faces the difficult task of identifying the regions where the combined fluorescence due to multiple electric dipole (ED) transitions becomes negligible compared to the fluorescence of the MD transition. We have succeeded in identifying a number of configurations with dielectric sphere parameters and a radial position of a trivalent rare-earth emitter wherein the branching ratio of the MD transition approaches its limit of one, implying that transitions from a given initial level (e.g., 5D0^{5}\mathrm{D}_{0}5D0​ level of Eu3+{\mathrm{Eu}}^{3+}Eu3+) are completely dominated by the MD transition. The dimensionless directivity of the MD emission, the radiative decay rates, and the fluorescence of the magnetic light can be increased by a factor of more than 25, 103{10}^{3}103, and 104{10}^{4}104, respectively.