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arXiv:2402.00666 · Conference on Lasers and Electro-Optics Europe & European Quantum Electronics Conference (CLEO/Europe-EQEC)

Nanoscale Control over Magnetic Light-Matter Interactions

Benoît Reynier, Éric Charron, Obren Markovic, Bruno Gallas, Alban Ferrier, Sébastien Bidault, Mathieu Mivelle

Published Jun 23, 2025• 0 citations
arXivHTMLPDF

Abstract

Light-matter interactions are often considered driven by the electric optical field alone, ignoring the magnetic component of light. However, this magnetic component plays a key role in many optical processes, such as chiral light-matter interactions, ultrasensitive detection, enhancement of Raman optical activity, photon-avalanching, or forbidden photochemistry, which makes the manipulation of magnetic processes extremely important. For instance, it was demonstrated in Eu3+ ions that magnetic emission could be manipulated by tuning the local magnetic quantum environment surrounding magnetic dipoles by means of dielectric or plasmonic nanostructures [1], [2]. Along the same line, it is also possible to manipulate the electric and magnetic excitation of these ions by controlling the electric and magnetic fields distribution of the excitation light [3].

DOI
10.1109/cleo/europe-eqec65582.2025.11110116

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Light-matter interactions are often considered driven by the electric optical field alone, ignoring the magnetic component of light. However, this magnetic component plays a key role in many optical processes, such as chiral light-matter interactions, ultrasensitive detection, enhancement of Raman optical activity, photon-avalanching, or forbidden photochemistry, which makes the manipulation of magnetic processes extremely important. For instance, it was demonstrated in Eu3+ ions that magnetic emission could be manipulated by tuning the local magnetic quantum environment surrounding magnetic dipoles by means of dielectric or plasmonic nanostructures [1], [2]. Along the same line, it is also possible to manipulate the electric and magnetic excitation of these ions by controlling the electric and magnetic fields distribution of the excitation light [3].
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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].
Most studies of light-matter interactions at optical frequencies primarily focus on the electric field (EF) interactions, often overlooking the contribution of the optical magnetic field (MF). The EF component of light interacts with electric dipole (ED) moments in matter approximately10510^{5}105times more strongly than the MF interacts with magnetic dipole (MD) moments. However, the spectral signatures of these weak (or “hidden”) MD transitions obey different selection rules from those governing the ED transitions, offering complementary insights into the properties of the investigated sample. Exclusive investigation of the MD transitions requires the spatial separation of the MF and the EF maxima within the region of interest, despite their intrinsic coupling dictated by Maxwell's equations. Such spatial separation can be achieved using standing wave geometries [1], dielectric resonators [2], or cylindrical vector laser beams (CVBs) [3]. A focused CVB with radial polarization (RPB) generates a ring-shaped intensity profile (Fig. 1b) and exhibits an axial EF component. In contrast, an azimuthally polarized beam (APB) (Fig. 1a) features a longitudinal MF component oscillating along the optical axis. The interaction of APB ultrashort pulses with tailored metallic apertures (antennas) results in additional MF enhancement via generation of oscillating ring currents within the metal [4]. In this work, we fabricated and experimentally validated a testbed for MD-exclusive optical spectroscopy based on aμm\mu \mathrm{m}μm-sized metallic antenna with a fluorescent nanostructure precisely positioned within the MF-dominated region. As a target material, we used Eu3+Y2O3compound, featuring a MD transition centred at 527.5 nm and an ED transition at 532 nm.
Summary form only given. Controlling the interaction of light and matter is the basis for diverse applications ranging from light technology to quantum information processing. Nowadays, many of these applications are based on nanophotonic structures. It turns out that the confinement of light in such nanostructures imposes an inherent link between its local polarization and its propagation direction, also referred to as spin-momentum locking of light [1]. Remarkably, this leads to chiral, i.e., propagation direction-dependent effects in the emission and absorption of light, and elementary processes of light-matter interaction are fundamentally altered. For example, when coupling plasmonic particles or atoms to evanescent fields, the intrinsic mirror symmetry of the particles' emission can be broken. In our group, we observed this effect in the interaction between single rubidium atoms and the evanescent part of a light field that is confined by continuous total internal reflection in a whispering-gallery-mode microresonator [2]. In the following, this allowed us to realize chiral nanophotonic interfaces in which the emission direction of light into the structure is controlled by the polarization of the excitation light [3] or by the internal quantum state of the emitter [4], respectively. Moreover, we employed this chiral interaction to demonstrate an integrated optical isolator [5] as well as an integrated optical circulator [6] which operate at the single-photon level and which exhibit low loss. The latter are the first two examples of a new class of nonreciprocal nanophotonic devices which exploit the chiral interaction between single quantum emitters and transversally confined photons.