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arXiv:2607.19832

Toroidal Transitions in Hydrogenic and Alkali Atoms

Kai Xiang Lee, Vincent Mancois, Kelvin Lim, David Wilkowski

physics.atom-phquant-phSubmitted Jul 22, 2026• Announced Jul 23, 2026• 0 citations
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Abstract

In addition to electric and magnetic multipoles, the expansion of current density also yields toroidal terms, a lesser-known family of multipoles. A recent proposal, I. Kuprov $\textit{et al.}$, Science Adv. 8 abq6751 (2022), explores the possibility of a direct observation of optical toroidal transitions in hydrogen and alkali atoms in the presence of a large magnetic field that decouples the spin and the angular momentum of the electron. However, the difficulty of observing these transitions against the nearby electric dipole (E1) transitions were underestimated because of extra admixture coming from diamagnetic coupling. Here, we revisit the toroidal coupling in atoms, taking diamagnetic contribution into account, and discuss the technical challenges of observing toroidal coupling in atomic physics. We show that toroidal transition should be searched in transitions with low principal quantum numbers. The remaining strong electric-dipole contribution could be removed using an appropriate differential measurement.

Comments
9 pages, 5 figures, 1 table

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In addition to electric and magnetic multipoles, the expansion of current density also yields toroidal terms, a lesser-known family of multipoles. A recent proposal, I. Kuprov et al.\textit{et al.}et al., Science Adv. 8 abq6751 (2022), explores the possibility of a direct observation of optical toroidal transitions in hydrogen and alkali atoms in the presence of a large magnetic field that decouples the spin and the angular momentum of the electron. However, the difficulty of observing these transitions against the nearby electric dipole (E1) transitions were underestimated because of extra admixture coming from diamagnetic coupling. Here, we revisit the toroidal coupling in atoms, taking diamagnetic contribution into account, and discuss the technical challenges of observing toroidal coupling in atomic physics. We show that toroidal transition should be searched in transitions with low principal quantum numbers. The remaining strong electric-dipole contribution could be removed using an appropriate differential measurement.
Introduction The selection rules discussed in Sec. 3.5 forbid many kinds of transitions that are frequently observed or exploited. It must be remembered that these “rules” are based on the approximations of Sec. 3.2, but of course, those can be extended. Such expansions to higher orders of approximation may seem to be little more than a tedious exercise, but this chapter will show that the results are extremely important, because they cause qualitatively different kinds of transitions. Since they involve both the electric and magnetic components of the light, their atomic dipole moments will be identified with the superscript E and B for the remainder of this chapter. The magnetic dipole transitions, called M1, discussed in Sec. 4.2.1 that arise from extension of the electric dipole approximation encompass all of magnetic resonance, including atomic clocks, forced evaporative cooling in Bose–Einstein Condensation (BEC), MRI, and astrophysical processes such as generation of the all-important 21 cm radio frequency line. The electric quadrupole transitions, called E2, discussed in Sec. 4.2.2 describe myriad stellar spectral features as well as the vast majority of nuclear γ-ray transitions. Even with these extensions there are many cases where the relaxation of the electric dipole (E1) selection rules to include M1 and E2 transitions as in Sec. 4.2 still do not account for observed processes. Thus other approximations have to be extended so that their limitations can be relaxed as well. Extension of the perturbation approximation (see Sec. 4.3.1) provides an analytical description of most of non-linear optics, including second harmonic generation, four wave mixing, Raman spectroscopy, and the fabled decay of the hydrogen 2S state. A semi-classical description of the interaction between radiation and atoms can begin with a multipole expansion of the Hamiltonian. The lowest-order term is just from the point charges α located at, and vanishes for neutral atoms. The next-order term is the electric dipole interaction that arises from the non-isotropic distribution of charges induced by the electric field of the light. This term produces the electric dipole transitions (E1) that have been described in some detail in Chap. 3.
This paper presents results for the anapole magnetic field moment due to the mixing of states with opposite parity in the n = 2 hydrogen atom in an external constant electric field. The evaluation of the current densities of the four n = 2 states is carried out to first order in the field strength. These current densities and their associated magnetic fields are expanded in multipoles, including both the ordinary poloidal and the toroidal fields. The dominant contribution to the toroidal dipole (anapole) magnetic field comes from the strong mixing of the degenerate 2S, 2P states within the n = 2 shell. A brief discussion is also presented of the electronic scattering from the anapole field of a Rydberg atom. The experimental conditions under which the atomic anapole field could be detected are critically considered, in particular, in terms of the quasi-resonant dependence of the anapole field on the applied electric field.
We report here the first observation and measurement of the transition magnetic moment for a strongly forbidden S-S transition of an alkali atom. By using single-photon excitation of the 6S1/2-7S1/2 caesium transition in a quasi-static electric field, we have detected an electronic polarization of the excited state, specific to an interference effect occurring in mixed electric magnetic dipole transitions. Our measurements, independent of the vapour density, indicate that the magnetic dipole amplitude M 1 has the same size as the electric dipole amplitude E1 , induced by an electric field, parallel to the light wave polarization, and equal to 2.62 ± 0.21 V/cm. We also obtain the relative sign of M 1 and E1. Using a theoretical value of E 1 and a well-defined phase convention, we deduce for the magnetic moment of the transition < 7S, 1/ 2 | μ z | 6S, 1/ 2 > = - (4.24 ± 0.34) 10-5 |μB|, in good agreement with a theoretical estimate. This result can also be expressed in terms of the oscillator strength in zero electric field f6S-7S = 4.05 × 10-15, or of the single-photon M1 decay rate Γ 7S-6S = 0.93 x 10-6 s-1.
We have discovered an interference which results in the vanishing of some electric dipole transition amplitudes. A transition-matrix element TTT between certain SSS and PPP sublevels with the same value of MF{M}_{F}MF​ vanishes when an applied magnetic field satisfies ${X}_{s}+{X}_{p}=\ensuremath{-}2{M}_{F}$, where $X={\ensuremath{\mu}}_{B}{g}_{J}\frac{B}{A}$, and AAA is the hfs constant. There must be an avoided crossing between the two states of the same MF{M}_{F}MF​ which can only occur when one of the hyperfine manifolds has an inverted Zeeman effect. These conditions imply MF<0{M}_{F}<0MF​<0 and I>JI>JI>J. We observed the vanishing of TTT in 23Na^{23}\mathrm{Na}23Na for one of the $\ensuremath{\Delta}{M}_{F}=0$ optical transitions of the $3{S}_{\frac{1}{2}}(F=1)\ensuremath{\rightarrow}3{P}_{\frac{1}{2}}(F=1)$ manifold. Absorption of cw laser light was monitored by observing total fluorescence perpendicular to both the atomic and laser beams, and absorption vanished near an applied field of 155 G. TTT vanishes for a large number of cases including rf and microwave frequencies and is a rather general consequence of angular momentum selection rules and perturbation theory. This phenomenon may have application in optical pumping, Lamb-shift measurements, and atomic weak neutral-current experiments.
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].