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arXiv:1404.5109 · Optics Letters

Wide-angle energy-momentum spectroscopy

Christopher M. Dodson, Jonathan A. Kurvits, Dongfang Li, Rashid Zia

Published Jun 24, 2014• 17 citations
arXivHTMLPDF

Abstract

Light emission is defined by its distribution in energy, momentum, and polarization. Here, we demonstrate a method that resolves these distributions by means of wide-angle energy-momentum spectroscopy. Specifically, we image the back focal plane of a microscope objective through a Wollaston prism to obtain polarized Fourier-space momentum distributions, and disperse these two-dimensional radiation patterns through an imaging spectrograph without an entrance slit. The resulting measurements represent a convolution of individual radiation patterns at adjacent wavelengths, which can be readily deconvolved using any well-defined basis for light emission. As an illustrative example, we use this technique with the multipole basis to quantify the intrinsic emission rates for electric and magnetic dipole transitions in europium-doped yttrium oxide (Eu³⁺:Y₂O₃) and chromium-doped magnesium oxide (Cr³⁺:MgO). Once extracted, these rates allow us to reconstruct the full, polarized, two-dimensional radiation patterns at each wavelength.

DOI
10.1364/ol.39.003927

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Light emission is defined by its distribution in energy, momentum, and polarization. Here, we demonstrate a method that resolves these distributions by means of wide-angle energy-momentum spectroscopy. Specifically, we image the back focal plane of a microscope objective through a Wollaston prism to obtain polarized Fourier-space momentum distributions, and disperse these two-dimensional radiation patterns through an imaging spectrograph without an entrance slit. The resulting measurements represent a convolution of individual radiation patterns at adjacent wavelengths, which can be readily deconvolved using any well-defined basis for light emission. As an illustrative example, we use this technique with the multipole basis to quantify the intrinsic emission rates for electric and magnetic dipole transitions in europium-doped yttrium oxide (Eu³⁺:Y₂O₃) and chromium-doped magnesium oxide (Cr³⁺:MgO). Once extracted, these rates allow us to reconstruct the full, polarized, two-dimensional radiation patterns at each wavelength.
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.
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].
A density-matrix approach has been developed for the angular distribution and polarization of radiative emission during single-photon atomic transitions for a general set of steady-state excitation processes in an arbitrary arrangement of static (or quasistatic) electric and magnetic fields. Particular attention has been directed at spectroscopic observations in the intense fields of the high-power ion diodes on the Particle Beam Fusion Accelerator II (PBFA II) and SABRE devices at Sandia National Laboratories and at magnetic-field measurements in tokamak plasmas. The field-dependent atomic eigenstates are represented as expansions in a complete basis set of field-free bound and continuum eigenstates. Particular emphasis has been given to directed-electron collisional excitations, which may be produced by an anisotropic incident-electron velocity distribution. We have allowed for the possibility of the coherent excitation of the nearly degenerate field-dependent atomic substates, which can give rise to a complex spectral pattern of overlapping Stark-Zeeman components. Coherent excitations may be produced by a beam of electrons that are spin-polarized at an angle with respect to the propagation direction or by nonparallel electric and magnetic fields. Our main result is a general expression for the matrix elements of the photon-polarization density operator representing the total intensity, angular distribution, and polarization of the atomic radiative emission. For the observation of radiative emission in the direction of the magnetic field, the detection of linearly polarized emission, in addition to the usual circularly polarized radiation, can reveal the presence of a perpendicular electric field or a coherent excitation mechanism.
Quantum gas microscopes are a promising tool to study interacting quantum many-body systems and bridge the gap between theoretical models and real materials. One of the most powerful experimental methods in solids is angle-resolved photoemission spectroscopy (ARPES), which measures the single-particle spectral function. The authors propose a measurement scheme to experimentally access the momentum- and energy-resolved spectral function in a quantum gas microscope. As an example for possible applications, the spectrum of a single hole excitation in one-dimensional ttt-JJJ models is calculated and analyzed. A sharp asymmetry in the distribution of spectral weight, reminiscent of the Fermi arcs observed in the pseudogap phase of cuprates, appears in the case of an isotropic Heisenberg spin chain.
From prehistoric times has come recognition that sunlight and firelight provide warmth, and that such illumination casts shadows. Expressed in more contemporary terms one would say that light travels in rays, and that this radiation has the potential to provide heat energy to absorbing material. From the time of Newton it has been known that light sources emit radiation comprising a distribution of colors. During the nineteenth century it was recognized that radiation had characteristics of transverse waves (with wavelength associated to color) but until the late twentieth century, when lasers became laboratory tools, it was hardly necessary to delve into the equations of electromagnetic theory to treat such experiments as were then possible; interest lay primarily with thermodynamic considerations of energy flow or with measurements of the dark or bright lines seen in the distribution of light that, after passing through a slit, was dispersed by a prism or grating into constituent colors. Although laser light sources are essential for the types of atomic excitation considered in this monograph, the legacy from thermal radiation still influences many interpretations of the interaction between radiation and matter, and it is therefore useful to summarize some of those concepts. The mathematics needed for describing laser radiation, or polarized light in general, has much in common with the mathematics of quantum theory discussed starting in Sec. 3.5 and specialized to two-level atoms in Sec. 5.6. In both cases one deals with two complex-valued functions – independent electric field amplitudes or probability amplitudes – whose absolute squares are measurable.