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.
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.
We experimentally quantify the contribution of magnetic dipole (MD) transitions to the near-infrared light emission from trivalent erbium-doped yttrium oxide (Er3+:Y2O3). Using energy-momentum spectroscopy, we demonstrate that the 4I${}_{13/2}{\ensuremath{\rightarrow}}^{4}$I15/2 emission near 1.5 $\ensuremath{\mu}$m originates from nearly equal contributions of electric dipole (ED) and MD transitions that exhibit distinct emission spectra. We then show how these distinct spectra, together with the differing local density of optical states for ED and MD transitions, can be leveraged to control Er3+ emission in structured environments. We demonstrate that far-field emission spectra can be tuned to resemble almost pure emission from either ED or MD transitions and show that the observed spectral modifications can be accurately predicted from the measured ED and MD intrinsic emission rates.
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].
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.
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 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.
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.
Due to the recent interest in magnetic light-matter interactions, the magnetic dipole (MD) transitions in lanthanide ions have been studied for potential applications in nano-optics. Similar to lanthanide ions, transition-metal ions also exhibit strong MD emission at room temperature, but their prominent MD zero-phonon lines are often accompanied by significant electric dipole (ED) sideband emission. Here, we extend energy-momentum spectroscopy to time-resolved measurements, and use this technique to quantify the ED and MD contributions to light emission from trivalent chromium doped magnesium oxide (Cr(3+):MgO). This allows us to differentiate the MD (2)E → (4)A2 zero-phonon line from phonon-assisted (2)E → (4)A2 and (4)T2 → (4)A2 ED sidebands. We also demonstrate how the relative intensities of the sharp MD zero-phonon line and the broad ED sidebands can be used as a qualitative measure of the MD and ED local density of optical states.