Rare-earth doped nanocrystals possess optical transitions with significant either electric or magnetic dipole characters. They are of considerable interest for understanding and engineering light-matter interactions at the nanoscale with numerous applications in nanophotonics. Here, we study the ${}^{5}{D}_{0}{\ensuremath{\rightarrow}}^{7}{F}_{1}$ transition dipole vector in individual ${\mathrm{NaYF}}_{4}:{\mathrm{Eu}}^{3+}$ nanorod crystals by Fourier and confocal microscopies. A single-crystal host matrix leads to narrow emission lines at room temperature that permit separation of the Stark sublevels resulting from the crystal-field splitting. We observe a fully magnetic transition and low variability of the transition dipole orientation over several single nanorods. We estimate the proportion of the dipole transitions for the Stark sublevels. We also determine an effective altitude of the rod with respect to the substrate. The narrow emission lines characteristic of ${\mathrm{NaYF}}_{4}:{\mathrm{Eu}}^{3+}$ ensure well-defined electric or magnetic transitions, and are thus instrumental for probing locally their electromagnetic environment by standard confocal microscopy.
Rare-earth doped nanocrystals possess optical transitions with significant either electric or magnetic dipole characters. They are of considerable interest for understanding and engineering light-matter interactions at the nanoscale with numerous applications in nanophotonics. Here, we study the 5D0\ensuremath→7F1 transition dipole vector in individual NaYF4:Eu3+ nanorod crystals by Fourier and confocal microscopies. A single-crystal host matrix leads to narrow emission lines at room temperature that permit separation of the Stark sublevels resulting from the crystal-field splitting. We observe a fully magnetic transition and low variability of the transition dipole orientation over several single nanorods. We estimate the proportion of the dipole transitions for the Stark sublevels. We also determine an effective altitude of the rod with respect to the substrate. The narrow emission lines characteristic of NaYF4:Eu3+ ensure well-defined electric or magnetic transitions, and are thus instrumental for probing locally their electromagnetic environment by standard confocal microscopy.
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.
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].
Engineering the local density of states with nanophotonic structures is a powerful tool to control light-matter interactions via the Purcell effect. At optical frequencies, control over the electric field density of states is typically used to couple to and manipulate electric dipole transitions. However, it is also possible to engineer the magnetic density of states to control magnetic dipole transitions. In this work, we experimentally demonstrate the optical magnetic Purcell effect using a single rare earth ion coupled to a nanophotonic cavity. We engineer a new single photon emitter, Er3+ in MgO, where the electric dipole decay rate is strongly suppressed by the cubic site symmetry, giving rise to a nearly pure magnetic dipole optical transition. This allows the unambiguous determination of a magnetic Purcell factor Pm=1040±30. We further extend this technique to realize a magnetic dipole spin-photon interface, performing optical spin initialization and readout of a single Er3+ electron spin. This work demonstrates the fundamental equivalence of electric and magnetic density of states engineering, and provides a new tool for controlling light-matter interactions for a broader class of emitters.
Elucidating magnetic structure with optical dopants: erbium-doped Gd2SiO5
The narrowness of the optical transitions of rare-earth-ion dopants makes them highly sensitive probes of their environment. We measured the optical transitions Er3+ dopants to determine the previously unknown magnetic ordering of Gd2SiO5 -- a promising host for quantum applications of rare-earth dopants. By measuring the transitions' magnetic-field dependence we determined an antiferromagnetic ordering with spins oriented along or slightly canted from the crystal's a∗ axis. The optical transitions are narrower than the coupling to gadolinium spins revealing information about the coupling strengths. We further optically measured a Néel temperature of 1.86±0.01stat.±0.07syst. K, and assembled a phase diagram in applied field and temperature showcasing a triple point where two gadolinium sites order semi-independently from each other. At high applied field the erbium dopants show long optical coherence times up to 0.4 ms at 3 T; at low fields these are probably limited by three low-frequency magnon modes below 10 GHz, observed directly. This study can be used to benchmark a method of magnetic structure determination.
Determining the local symmetry of luminescent centers in crystals is critical for understanding and controlling their optical transitions, yet current methods are limited by stringent experimental requirements and ambiguous symmetry assignments. Here, we develop a robust computational electromagnetics framework that directly connect the local symmetry and chirality of rare-earth-doped single crystals to the polarization states of their emitted light. This framework is experimentally validated through the precise determination of point and space group symmetries using high-resolution, polarization-resolved micro-photoluminescence (μ-PL) spectra. Unlike conventional approaches that usually rely on analyzing multiple transitions at cryogenic temperatures, our technique operates at room temperature, requires only a single optical transition, and enables accurate orientation of symmetry axes. This enables deterministic polarization control of nano-emitters by tailoring symmetry groups and selecting appropriate transition dipoles, eliminating the need for bulky or complex photonic structures. Additionally, we demonstrate the function of bio-sensing, via determining single particle orientations in complex cellular environments using minimal polarization measurements. These results pave the way for advances in energy transfer systems, ultra-bright rare-earth nanocrystals, nanophotonic materials, and real-time single-particle tracking in biological contexts.
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.