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High-Brightness Sources and Light-Driven Interactions

Spectrally Selective Excitation of Electric Dipole and Magnetic Dipole Transitions in Eu3+Y2O3 Nanostructures

Elizaveta Gangrskaia, Alessandra Bellissimo, Valentina Shumakova, Sarah Pulikottil Alex, I. Bugár, Lorenz Grünewald, Sebastian Mai, Thomas Schachinger, Dariusz Pysz, Ryszard R. Buczynski, Andrius Baltuška, Audrius Pugzlys

Published Jan 1, 2024• 0 citations
Publisher

Abstract

Implementing Stimulated Raman Scattering in a hollow-core fiber and spectral focusing in a long nonlinear crystal, we generate narrowband tunable ultrafast pulses for selective excitation of electric or magnetic dipole transitions in a FIB-fabricated Eu3+Y2O3 nanostructure.
DOI
10.1364/euvxray.2024.jtu4a.3

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High Resolution Image Download MS PowerPoint Slide At optical frequencies, interactions of the electric field component of light with matter dominate, whereas magnetic dipole transitions are inherently weak and challenging to access independently of electric dipole transitions. However, magnetic dipole transitions are of interest, as they can provide valuable complementary information about the matter under investigation. Here, we present an approach which combines structured light irradiation with tailored sample morphology for enhanced and high-contrast optical magnetic field excitation, and we test this technique on Eu 3+ ions. We generate spectrally tunable, narrowband, polarization-shaped ultrashort laser pulses, which are specifically optimized for the spectral and the spatial selective excitation of magnetic dipole and electric dipole transitions in Eu 3+:Y 2 O 3 nanostructures integrated into a metallic antenna. In the presence of the metallic antenna, the excitation with an azimuthally polarized beam is shown to provide at least a 3.0–4.5-fold enhancement of the magnetic dipole transition as compared to a radially polarized beam or a conventional Gaussian beam. Thus, our setup provides new opportunities for the spectroscopy of forbidden transitions.
Optical frequency magnetic dipole (MD) transitions follow different selection rules from those invoked by the coupling of light to the electric dipole (ED) moment giving valuable complementary spectral information about the system under investigation. However, MD interactions contribute to the optical spectrum by approximately two orders of magnitude less than the ED transitions, therefore remaining concealed in traditional optical spectroscopy. To allow the unperturbed direct detection of the magnetic-field-MD interactions a novel type of magneto-optical spectroscopy is proposed. To this end, spatial separation of the electric and the magnetic field (EF & MF) components of the light can be achieved by means of azimuthally polarised beams (APB) [1]. Under external focusing, the APB develops a doughnut-shaped intensity profile exhibiting a longitudinal MF component at the centre of the beam while the polarisation of the EF oscillates along the beam perimeter. Another way to discern between ED and MD transitions is through spectral selectivity. For example, Eu3+ ions exhibit a MD-allowed transition at 527.5 nm and an ED-allowed one at 532 nm [2].
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.
We use the magnetic field distribution of an azimuthally polarized focused laser beam to excite a magnetic dipole transition in Eu^{3+} ions embedded in a Y2O3 nanoparticle. The absence of the electric field at the focus of an azimuthally polarized beam allows us to unambiguously demonstrate that the nanoparticle is excited by the magnetic dipole transition near 527.5 nm. When the laser wavelength is resonant with the magnetic dipole transition, the nanoparticle maps the local magnetic field distribution, whereas when the laser wavelength is resonant with an electric dipole transition, the nanoparticle is sensitive to the local electric field. Hence, by tuning the excitation wavelength, we can selectively excite magnetic or electric dipole transitions through optical fields.
Naturally occurring magnetic dipole resonances can be used as optical sources in metamaterials and optical nanostructures to engineer light emission with applications in energy harvesting, biological imaging, and other photonic devices. Here, we use energy-momentum spectroscopy to quantify the electric and magnetic dipole emission rates of near-infrared transitions in Dy3+ and Tm3+ doped Y2O3. Of these emission lines, we find that the overlapping 4F9/2 → 6F11/2 and 4F9/2 → 6H9/2 transitions in Dy3+ and the overlapping 1G4 → 3H5 and 3H4 → 3H6 transitions in Tm3+ exhibit the greatest MD emission and thus offer the most direct pathway for integration with magnetic modes in resonant nanostructures.