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Physical Review Letters

Spectral Tuning by Selective Enhancement of Electric and Magnetic Dipole Emission

Sinan Karaveli, Rashid Zia

Published May 11, 2011• 173 citations
Publisher

Abstract

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.

DOI
10.1103/physrevlett.106.193004

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The Purcell effect is commonly used to increase light emission by enhancing the radiative decay of electric dipole transitions. In this Letter, we demonstrate that the opposite effect, namely, the inhibition of electric dipole transitions, can be used to strongly enhance light emission via magnetic dipole transitions. Specifically, by exploiting the differing symmetries of competitive electric and magnetic dipole transitions in trivalent europium, we demonstrate a fourfold enhancement of the far-field emission from the (5)D(0)→(7)F(1) magnetic dipole transition in trivalent europium. We show that this strong enhancement is well predicted by a three-level model that couples the individual Purcell enhancement factors of competitive transitions from the same excited state.

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Conference on Lasers and Electro-Optics•Jan 1, 2009•0 citations
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.
The Purcell effect is commonly used to increase light emission by enhancing the radiative decay of electric dipole transitions. In this Letter, we demonstrate that the opposite effect, namely, the inhibition of electric dipole transitions, can be used to strongly enhance light emission via magnetic dipole transitions. Specifically, by exploiting the differing symmetries of competitive electric and magnetic dipole transitions in trivalent europium, we demonstrate a fourfold enhancement of the far-field emission from the (5)D(0)→(7)F(1) magnetic dipole transition in trivalent europium. We show that this strong enhancement is well predicted by a three-level model that couples the individual Purcell enhancement factors of competitive transitions from the same excited state.
Summary form only given. Although it is often assumed that all light-matter interactions at optical frequencies are mediated by electric dipole transitions, strong optical-frequency magnetic dipoles do exist. In fact, we see magnetic dipole emission every day from the many lanthanide ions (such as erbium, europium, and terbium) that help to illuminate everything from fluorescent lighting to telecom fiber amplifiers. Higher-order processes such as magnetic dipole and electric quadrupole transitions also play an important part in the light emission from transition metal ions and semiconductor quantum dots. Nevertheless, most applications have overlooked the device implications of these electric-dipole-forbidden transitions throughout the visible and near-infrared regime, and their contributions to many important emitters have not been fully characterized.In this presentation, we will experimentally characterize the "forbidden" transitions in a range of solid-state emitters and investigate their applications and implications for nanophotonics. We will examine the electric dipole approximation commonly used to describe light-matter interactions and discuss naturally occurring systems that exhibit higher-order magnetic dipole and electric quadrupole emission. We will illustrate how these nanoscale quantum transitions can provide both a new way to probe magnetic light-matter interactions and a new degree of design freedom for active electronic and photonic devices. Specifically, we will demonstrate how the different symmetries of multipolar transitions can be exploited to identify, quantify, and control light emission, even at sub-lifetime scales. Despite similar radiation patterns, magnetic and electric dipole emitters have different symmetries with respect to polarization and phase. Thus, in an inhomogeneous environment, we can tailor interference effects and the local density of optical states to selectively enhance either electric or magnetic dipole emission [1,2]. To examine the scope of such higher-order transitions, we will present quantum mechanical calculations that identify all the magnetic dipole and electric quadrupole emission lines in the trivalent lanthanide series in the visible to near-infrared spectrum [3]. Then, we will present an energyand momentum-resolved spectroscopy technique to directly quantify the electric and magnetic dipole contributions from any mixed transition. [4] Using energy-momentum spectroscopy, we will experimentally examine the higher order transitions in lanthanide ions [4,5], transition metal ions [6], and epitaxial quantum dots [7]. If time permits, we will then show how the symmetry differences between magnetic and electric dipoles can be used to address specific electronic states [6] and to dynamically tune emission spectra at sub-lifetime-scales [8].
Radiative transition rates are known to be tunable by changing the photonic environment of a fluorescent species. In this work, we investigate the influence of nearby metallic interfaces on the transition rates of Eu3+ ions. Specifically, we consider the magnetic dipole (MD) and electric dipole (ED) transitions that are visible in the luminescence spectrum of Eu3+ ions, which respond differently to a change in the photonic environment. Three different fabrication processes were used to prepare layered substrates with Eu3+ at a variable distance above a gold or silver mirror, or sandwiched between two gold or silver mirrors.\n\nA complete theoretical description of these layered substrates, using a Dyadic Green's formalism, is presented, leading to a set of directly applicable formulae. These formulae were found to provide very accurate predictions of the single mirror system spectra. The photoluminescence lifetimes of Eu3+ in these systems could not be reproduced: different factors seem to play a role here.\n\nThe quality of the emitting layer was found to have a significant effect on the fluorescence behaviour. A scattering emitting layer causes the emission coherence to be lost quickly, giving unpredictable results. Thermal treatment results in a very clear emitting layer, but emission brightness is reduced up to the point where no reliable spectrum could be recorded anymore for double mirror systems. Better control over the fabrication of the emitting layer is needed.
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.
Abstract Absorption and emission in the ultraviolet, visible, and infrared spectral range are usually mediated by the electric-field component of light. Only some electronic transitions have significant “magnetic-dipole” character, meaning that they couple to the magnetic field of light. Nanophotonic control over magnetic-dipole emission has recently been demonstrated, and magnetic-dipole transitions have been used to probe the magnetic-field profiles of photonic structures. However, the library of available magnetic-dipole emitters is currently limited to red or infrared emitters and mostly doped solids. Here, we show that NaYF4 nanocrystals doped with Eu3+ have various electric- and magnetic-dipole emission lines throughout the visible spectral range from multiple excited states. At the same time, the colloidal nature of the nanocrystals allows easy handling. We demonstrate the use of these nanocrystals as probes for the radiative electric and magnetic local density of optical states in a planar mirror geometry. A single emission spectrum can reveal enhancement or suppression of the density of optical states at multiple frequencies simultaneously. Such nanocrystals may find application in the characterization of nanophotonic structures or as model emitters for studies into magnetic light–matter interaction at optical frequencies.