The electromagnetic-vacuum-field fluctuations are intimately linked to the process of spontaneous emission of light. Atomic emitters cannot probe electric- and magnetic-field fluctuations simultaneously because electric and magnetic transitions correspond to different selection rules. In this Letter we show that semiconductor quantum dots are fundamentally different and are capable of mediating electric-dipole, magnetic-dipole, and electric-quadrupole transitions on a single electronic resonance. As a consequence, quantum dots can probe electric and magnetic fields simultaneously and can thus be applied for sensing the electromagnetic environment of complex photonic nanostructures. Our study opens the prospect of interfacing quantum dots with optical metamaterials for tailoring the electric and magnetic light-matter interaction at the single-emitter level.
The electromagnetic-vacuum-field fluctuations are intimately linked to the process of spontaneous emission of light. Atomic emitters cannot probe electric- and magnetic-field fluctuations simultaneously because electric and magnetic transitions correspond to different selection rules. In this Letter we show that semiconductor quantum dots are fundamentally different and are capable of mediating electric-dipole, magnetic-dipole, and electric-quadrupole transitions on a single electronic resonance. As a consequence, quantum dots can probe electric and magnetic fields simultaneously and can thus be applied for sensing the electromagnetic environment of complex photonic nanostructures. Our study opens the prospect of interfacing quantum dots with optical metamaterials for tailoring the electric and magnetic light-matter interaction at the single-emitter level.
One of the central assumptions in quantum electrodynamics is to invoke the dipole approximation because (quantum) emitters are much smaller than the wavelength of light. The main consequence is that only the electric dipole plays a role in light-matter interactions at optical frequencies. In this paper we show that semiconductor quantum dots possess large magnetic-dipole and electric-quadrupole moments, which can be accessed with light. Moreover, quantum dots are capable of mediating electric-dipole, magnetic-dipole and electric-quadrupole interactions on dipole-allowed transitions and therefore are fundamentally different than atoms.
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.
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].
The photonic environment can significantly influence emission properties and interactions among atomic systems. In such scenarios, frequently the electric dipole approximation is assumed that is justified as long as the spatial extent of the atomic system is negligible compared to the spatial variations of the field. While this holds true for many canonical systems, it ceases to be applicable for more contemporary nanophotonic structures. To go beyond the electric dipole approximation, we propose and develop in this article an analytical framework to describe the impact of the photonic environment on emission and interaction properties of atomic systems beyond the electric dipole approximation. Particularly, we retain explicitly magnetic dipolar and electric quadrupolar contributions to the light-matter interactions. We exploit a field quantization scheme based on electromagnetic Green’s tensors, suited for dispersive materials. We obtain expressions for spontaneous emission rate, Lamb shift, multipole-multipole shift and superradiance rate, all being modified with dispersive environment. The considered influence could be substantial for suitably tailored nanostructured photonic environments, as demonstrated exemplarily.
The photonic environment can significantly influence emission properties and interactions among atomic systems. In such scenarios, frequently the electric dipole approximation is assumed that is justified as long as the spatial extent of the atomic system is negligible compared to the spatial variations of the field. While this holds true for many canonical systems, it ceases to be applicable for more contemporary nanophotonic structures. To go beyond the electric dipole approximation, we propose and develop in this article an analytical framework to describe the impact of the photonic environment on emission and interaction properties of atomic systems beyond the electric dipole approximation. Particularly, we retain explicitly magnetic dipolar and electric quadrupolar contributions to the light-matter interactions. We exploit a field quantization scheme based on electromagnetic Green's tensors, suited for dispersive materials. We obtain expressions for spontaneous emission rate, Lamb shift, multipole-multipole shift and superradiance rate, all being modified with dispersive environment. The considered influence could be substantial for suitably tailored nanostructured photonic environments, as demonstrated exemplarily.
In 1946, E. M. Purcell predicted that the radiative lifetime of an emitter is not an intrinsic property but can be modified by structuring the surrounding electromagnetic field [36]. By inserting a semiconductor quantum dot (QD) in an optical cavity, one can accelerate or inhibit its spontaneous emission. In the present article, we show that the QD spontaneous emission can be deterministically controlled to fabricate bright sources of quantum light. QDs in cavities: basics, motivation, first demonstrations Light-matter coupling We note f the ground state of the QD and e its excited state. For a cavity mode close to resonance with the QD optical transition, we consider only the states with 0 or 1 photon in the cavity mode. The states ∣ e, 0〉 and ∣ f, 1〉 are coupled through light–matter interaction, with a constant g , where h g = ∣〈 e, 0∣ Ed ∣ f, 1∣, with d the dipole of the optical transition e → f and E the electric field at the QD position. Each of the states ∣ e, 0 > and ∣ f, 1 > are also coupled to continua of states: continuum of the free-space optical mode, phonons of the semiconductor matrix, etc. [4]. Here, we consider only the coupling to the continuum of the free-space optical mode, related to the cavity losses, with a constant γ c . When g << γ c , the photon emitted by the recombination of an exciton efficiently escapes outside the cavity. The QD optical transition radiative recombination rate can be accelerated (Purcell effect) or inhibited.