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10 1038/nmat4563
10 1038/nmat4563
10 1038/nmat4563
T
he interactions of electromagnetic radiation with matter under- Static toroidal multipoles
pin some of the most important technologies today — from Initially, the static toroidal dipole (or anapole) was introduced
telecommunications to information processing and data stor- as a configuration of static currents flowing on the surface of a
age; from spectroscopy and imaging to light-assisted manufacturing. torus6 (Fig. 1). It was pointed out that the external field of such a
Our understanding and description of the electromagnetic proper- configuration is identically zero, whereas the currents create a mag-
ties of matter traditionally involves the concept of electric and mag- netic field confined within the torus; hence static toroidal dipoles
netic dipoles, as well as their more complex combinations, known as do not interact directly with electric and magnetic fields6. The con-
multipoles. Introduced by Maxwell and Lorentz and later refined by cept of the anapole was later generalized to a full family of toroidal
Jackson, Landau and Lifshitz, this framework, termed the multipole multipoles and applied to the description of condensed matter 3,17.
expansion, is central in physics and is being routinely applied in the Toroidal ordering in the solid state was first investigated theoreti-
study of optical, condensed-matter, atomic, nuclear phenomena and cally in 1946 by Charles Kittel in his work on ferromagnetic domains
beyond1. Within this framework, electromagnetic media can be rep- of small particles18 and experimentally in 197419, followed by a series
resented by a set of point-like multipole sources2–5. The commonly of observations in 1984 and 1985, which confirmed the existence of
used set of multipoles comprises the electric and magnetic families, static toroidal moments20,21 (see also ref. 22 and references therein).
which can be represented by oscillating charges and loop currents Historically, two sets of toroidal multipoles have been considered in
respectively. Dynamic toroidal multipoles constitute a third inde- this context, termed toroidal electric (or axial) and toroidal mag-
pendent family of elementary electromagnetic sources, rather than netic (or polar)2. The first set arises from vortex-like configurations
an alternative multipole expansion or higher-order corrections to of electric dipoles2, whereas the latter set arises from currents flow-
the conventional electric and magnetic multipoles (Box 1). ing on the surfaces of tori, along the meridians or, equivalently, from
Introduced in 1957 by Y. B. Zeldovich6, toroidal moments have vortex-like configurations of magnetic dipoles (Fig. 2). Similarly,
been considered in systems of toroidal topology (Fig. 1) and stud- the family of electric (magnetic) toroidal multipoles can be gener-
ied in the context of nuclear 7, atomic8 and molecular physics9, ated by magnetic (electric) charge currents. However, since mag-
classical electrodynamics10,11 and solid state physics3. In the field netic charge currents do not exist, electric toroidal multipoles do
of electromagnetism, in particular, a number of works have led to not enter the multipole expansion2.
the development of a complete theoretical framework for toroidal Toroidal multipoles enter the description of condensed matter
electrodynamics12–16 and the prediction of exotic effects, including by an order parameter, termed toroidization or toroidal polariza-
dynamic non-radiating charge-current configurations11 and non- tion, analogous to the macroscopic electric polarization and mag-
reciprocal interactions10. Following recent experimental observa- netization23. Where electric polarization accounts for the electric
tions of toroidal contributions in the response of materials across the dipole density, and magnetization for magnetic dipole density,
electromagnetic spectrum, dynamic toroidal multipoles are now the toroidization represents the density of toroidal dipoles. A macro-
focus of substantial research efforts. Here, we will trace the develop- scopic toroidization emerges from configurations of local toroidal
ment of toroidal electrodynamics from the early considerations of moments that exhibit long-range order 24. Media that can exhibit
static toroidal moments in condensed matter, to the recent experi- macroscopic toroidization are called ferrotoroids, on equal footing
mental works on dynamic toroidal multipoles. We will examine the with ferroelectrics and ferromagnets. Whereas ferroelectrics break
way by which toroidal multipoles enter the description of the mate- spatial inversion symmetry and ferromagnets break time-reversal
rials’ response, a topic of ongoing discussion, and review advances symmetry, ferrotoroids with magnetic toroidization simultaneously
in the studies of the peculiar radiation properties of toroidal dipoles, break time-reversal and spatial inversion symmetry. Ferrotoroids
as well as the free-space propagating toroidal excitations. with effective electric toroidization formed by a loop of electric
Optoelectronics Research Centre & Centre for Photonic Metamaterials, University of Southampton, Highfield SO17 1BJ, UK. 2TPI and Centre for Disruptive
1
Photonic Technologies, Nanyang Technological University, Singapore 637378, Singapore. *e-mail: n.papasimakis@soton.ac.uk
Dynamic toroidal multipoles constitute an independent family of dipole moment oscillates at frequency ω (T(t)eiωt), its intensity
elementary electromagnetic sources. In the absence of intrinsic has an additional scaling factor k 2 = ω2/c 2 as compared to the
magnetization, toroidal multipoles complete the standard dynamic electric dipole16:
multipole expansion comprising the conventional electric and mag-
netic multipoles (Fig. 2). More specifically, they represent the scat- IT = 2-3 ck 4|kT|2
tering contributions of oscillating radial currents J (that is r ∙ J ≠ 0)
and hence are different in nature from the electric and magnetic which, in principle, allows one to disentangle toroidal and elec-
multipoles associated with oscillating charge density and transverse tric dipole emissions via spectroscopic analysis5,16. Moreover, the
currents (r × J ≠ 0), respectively. In particular, the lowest order toroi- vector potential, AT(r,t), of the toroidal emission differs from the
dal multipole, the toroidal dipole, corresponds to currents flowing vector potential, Ap(r,t), emitted by an electric dipole, and, in fact,
on the surface of an imaginary torus, along its meridians (Fig. 2). Its their difference ΔA = AT – Ap cannot be eliminated via a gauge
moment T is directed along the axis of the torus and is given by 3,16: transformation14. Indeed, the electromagnetic fields emitted by a
point-like toroidal dipole, superimposed with a point-like electric
T=−1
0c ∫ d
1−
3r [r(r·J) − 2r2J]
dipole p = ikT vanish at any distance away from the source (but
not at the source), whereas the corresponding vector potential
where c is the speed of light. Importantly, the toroidal dipole fea- remains nonzero88:
tures neither charge poles (since it is a purely current excitation),
ΔA=(T·(−−r− )
−ikr
nor magnetic poles where magnetic field lines seem to diverge or e
) +4πδ (3)(r)T
converge. Furthermore, the toroidal dipole interacts directly only
with external conduction (Jext) and displacement currents (∂D/∂t) where δ(3)(r) is the three-dimensional delta function. Since all
or, equivalently, with a vortex of magnetic field ( × B), as it fol- effects of gauge-fixing can be described by addition of a gradient
lows from the expression for the energy of its interaction with of an arbitrary function, f, to the vector potential, the non-trivial
electromagnetic fields12 (for a comparison with the electric and part of the vector potential, irremovable by gauge-fixing, will be
magnetic dipole terms, see Table 1): given by terms with nonzero curl:
In particular, in the static case, the toroidal dipole interacts It follows that the second term in the expression for the net
only with conduction currents, and tends to align parallel to the vector potential does not vanish upon application of the curl,
current flow. which indicates that net vector potential cannot be eliminated at
Despite being physically distinct from the electric dipole, the all points in space in any gauge, and is therefore non-trivial.
toroidal dipole emits radiation with the same angular momen- We would like to note that in the current and following Box 2,
tum and parity properties as the former 5,14, and therefore the we employ a Gaussian unit system, in accordance with the major-
two multipoles cannot be distinguished by a distant observer. ity of works on the topic of toroidal electrodynamics. Simple
Nevertheless, the toroidal dipole emission presents a distinct fre- means to convert the relations reported here to SI units can be
quency dependence, and in the harmonic case where the toroidal found in ref. 89.
dipoles, on the other hand, appear invariant under both time and Dynamic toroidal multipoles
space inversions25–27. Ferrotoroids will exhibit electric polarization For simplicity we will refer to magnetic toroidal moments as toroi-
(magnetization) in response to an external magnetic (electric) field. dal in this section. Dynamic toroidal multipoles can be induced by
This magnetoelectric response is expected to form the basis for and interact with oscillating electromagnetic fields, and thus con-
applications in technological areas, such as data storage, where for tribute to the optical properties of materials across the entire electro
example an electric field can read or write information in the mag- magnetic spectrum3. However, the inclusion or omission of the
netic state of a medium28,29. In addition, ferrotoroids are expected to dynamic toroidal multipoles from the multipole expansion is the
exhibit unique forms of magnetic response30–32 and nonreciprocal subject of an ongoing discussion45–47, in particular with respect to
reflection and dichroism17. their appearance in equivalent descriptions, such as Mie theory 48,49.
At present, the range of static toroidal systems under study We address this in detail in a dedicated section (Box 2) illustrating
includes various compounds33,34 such as boracites35, pyroxenes36 that although both the vector spherical harmonic Mie expansion and
and olivines37; metals38; glasses39; ferroelectric nanoscale disks and the (full, including toroidal contributions) charge-current multipole
rods26; and molecular magnets40,41. However, unambiguous observa- expansion are complete, the toroidal multipoles appear explicitly
tions of long-range toroidal order have proven challenging due to in the charge-current multipole, whereas their presence in the Mie
the weak, short-range interactions between toroidal dipoles and the expansion is inexplicit. The importance of toroidal multipoles for
requirement of demonstrating both space- and time-reversal sym- light–matter interactions has direct implications for the interpreta-
metry breaking to prove its existence17. Early experiments focused tion of electromagnetic excitation spectra and optical forces in media
on the magnetoelectric effect 42,43, which is not unique to the toroidal with constituents of toroidal topology and justifies the consideration
moments27, therefore these only provided an indication for ferro- of toroidal moments as a separate family of multipoles.
toroidic order. Subsequent experiments reported direct observa- Although observations of dynamic toroidal excitations are often
tions of ferrotoroidicity, where ferrotoroidic domains were observed complicated by the contributions of the electric and magnetic
in an olivine crystal (LiCoPO4) and domain orientations were iden- multipoles to the material response, they show up strongly in large
tified by second harmonic generation25. These findings were con- molecules or molecules with toroidal symmetry. Indeed, the scat-
firmed in follow-up works demonstrating hysteretic effects by a tering of electromagnetic waves by electric, magnetic and toroidal
similar nonlinear optical method44. dipole moments scales as ~(R/λ), ~(R/λ)2 and ~(R/λ)3, respectively,
90°
6.7 nm
Magnetic field
10.5 nm
5 fm 10 nm 1 µm+ Size
1 nm 0.1−1 µm
~300 nm
Figure 1 | Toroidal structures at different length scales. Toroidal topology, encountered very often in both artificial and naturally occurring objects, provides
an indication for the presence of spontaneous or induced toroidal moments. Top row, from left to right: solenoidal currents lead to a toroidal moment in the
atomic nucleus6; quaternary structure of archaeon (S. solfataricus) Cas4 (ref. 84); red blood cells take a biconcave, torus-like shape. Bottom row from left to
right: benzene (left), hexaphenylbenzene (centre) and a toroidal carbon cage consisting of 120 carbon atoms (right) are organic molecules with elements of
toroidal symmetry; perovskite (BaTiO3) nanotori87 are examples of artificial toroidal structures. Figure reproduced from: top row, middle, ref. 84, American
Chemical Society; top row, right, © PhonlamaiPhoto/iStock/Thinkstock; bottom row, left, cage image, ref. 9, APS; bottom row, right, ref. 87, APS.
Table 1 | Electric, magnetic, and toroidal dipole moments (p, m, T), interaction energy (W) with an electromagnetic field, and radiated
power (expressed as the radial component of the Poynting vector S) for the three multipole families.
Multipole family Dipole moment Interaction energy Far-field radiation patterns
W = ∫ d 3r ( ρφ − 1-J·A
c ) (r·S)
Electric p=−
iω ∫ d
1 3r J
–p·E−1-−∂
c ∂t (p·A) −
4−
ω4
π−
c3
|p| 2 (1 − (r·p)2)
|m| 2 (1 − (r·m
)2)
4
m=− 3r (r×J) –m·B ω
2c ∫ d
1
Magnetic −
4−
π−
c3
·
|T| 2 (1 − (r·T )2)
ω6
Toroidal T=−0c ∫ d
1
1−
3r [r(r·J) − 2r2J] –T·(D + 4πJ)/c −
4−
π−
c5
ρ, charge density; J, current density; φ, scalar potential; A, vector potential; vectors with hats denote the corresponding unit vectors.
where R is the characteristic length scale of the molecule and λ is the Toroidal response in artificial media
free-space wavelength14,16,50. Hence, the toroidal response of a system Metamaterials, artificial media periodically structured at the sub-
will become increasingly important, in comparison to the standard wavelength scale in order to achieve desirable electromagnetic
dipoles, as the size of the system or molecule increases. Relatively functionality, served as a platform for the first observation of
large molecules with R ≤ λ, such as artificial ‘metamolecules’, can resonances due to induced toroidal dipoles. Early works on toroi-
be found in man-made metamaterials. A metamaterial of toroidal dal metamaterials predicted the presence of backward waves and
topology can be engineered in such a way that excitation of the negative refraction in such material systems53. Experimental signa-
lower-order electric and magnetic multipoles is suppressed due to tures of a toroidal dipole response were first seen in the microwave
symmetry, thus allowing the toroidal dipole to become the leading dichroism spectra of chiral toroidal solenoid arrays in 200954, they
term in the multipole expansion and to contribute strongly to the were, however, obscured by the presence of dipole and higher-order
electromagnetic properties of the metamaterial51. Moreover, even electric and magnetic multipoles. The first observation of an iso-
when scattering contributions of the conventional multipoles are lated toroidal dipole absorption resonance was reported in 201051
dominant, the toroidal response of the nanostructures might still in a metamaterial whose metamolecules were formed by a ring-
be detected through optical forces49. Even for small, deeply sub- shaped arrangement of microwave resonators (Fig. 3a). In this type
wavelength systems, such as atoms and molecules, one can expect of metamaterial, excitation at the resonance frequency induces a
that toroidal dipole transitions could be observable, as they are of loop chain of oscillating magnetic dipole moments due to a com-
the same order as, for instance, magnetic quadrupole transitions52, bination of retardation effects and electromagnetic interactions
which are experimentally accessible. between individual resonators. The induced magnetic dipoles trace
Dipoles Charge
Current
Quadrupoles
Octupoles
Figure 2 | The ‘multipole zoo’. Electric multipoles represent charge configurations (far left column), whereas magnetic multipoles correspond to current
sources (second column from left). The (magnetic) toroidal multipole family (second column from the right) corresponds to current distributions that
cannot be represented by electric and magnetic multipoles. Same order members of each multipole family have identical power radiation patterns of
corresponding oscillating multipoles (far right column). Electric and toroidal dipoles also have identical radiated field patterns as indicated by the same
colour (red) arrows. Figure reproduced from ref. 50, APS.
the circumference of a closed loop leading to a field structure sim- Radiating properties of toroidal multipoles
ilar to that of a toroidal solenoid. These initial observations were The recent observations of toroidal dipole excitations in meta
quickly followed by works aiming to further enhance the toroidal materials have further stimulated the study of their radiation
response and suppress the contributions of competing electric and properties. Whereas the charge-current configurations and the cor-
magnetic multipoles55,56. responding near-field patterns of toroidal dipole modes are drasti-
Quasi-planar designs were considered57,58 (Fig. 3b) in an effort cally different from their electric dipole counterparts, the respective
to simplify the fabrication of toroidal metamaterials. By scal- far-field radiation patterns are virtually identical, apart from a phase
ing down the size of metamolecules based on clusters of split- factor (Fig. 2). The similarities of radiation properties have lead to
ring resonators, the toroidal response at terahertz59 and optical the suggestion of incorporating the electric and toroidal multipoles
frequencies60,61 (Fig. 3c) has been unambiguously detected. In into a single family72. However, the toroidal dipole far-field radia-
parallel, fabrication difficulties were also overcome by introduc- tion can be distinguished from the electric dipole radiation by its
ing artificial patterns that are less challenging to manufacture at dependence on frequency and permittivity of the dielectric environ-
the nanoscale, where split-ring resonators are replaced by pairs ment53. A considerable amount of literature exists that shows how
of bars62 (Fig. 3d) and disks63,64, while still supporting toroidal toroidal multipoles emerge as a third and independent family in the
excitation modes. In the optical part of the spectrum, a toroidal multipole expansion3,4,5,12,16. Thus, dynamic toroidal multipoles shall
dipole response, although damped by ohmic losses in metals, was be treated on equal footing with the dynamic electric and magnetic
found in even simpler systems, such as plasmonic core-shell nano multipoles and indeed, charge-current configurations of exclusively
particles65, and bas-relief patterns that support spoof plasmons, electric, magnetic and toroidal character exist13,14 (see also Box 2).
including periodic grids66 and arrays of ring-shaped grooves illu- Toroidal dipole emitters can be combined with electric dipole
minated at oblique angles67 (Fig. 3e). A toroidal response was also emitters where the radiated fields interfere destructively11,15,16. Such
observed in plasmonic void oligomers using energy-loss trans- a non-radiating configuration is in fact a dynamic version of the
mission electron microscopy 68 (Fig. 3f). Finally, recent studies of anapole14. The dynamic anapole was first observed in a microwave
toroidal excitations moved towards novel laser emitters69, and low- metamaterial73 (Fig. 3h). It was also shown that the destructive
loss nanostructured dielectric70 (Fig. 3g) and superconducting 58 interference between coherently oscillating electric and toroi-
material structures. dal dipoles provides a new mechanism of electromagnetic trans-
The link between the dynamic microscopic toroidal response and parency that yields narrow and symmetric transparency lines.
directly observable macroscopic quantities (such as material trans- Similar resonances were recently detected in the scattering spectra
mission, reflection and absorption) has been investigated in a series of dielectric nanoparticles48 (Fig. 3i) and were also predicted for
of works, but the discussion on the form of the constitutive equations core-shell wires74 and hybrid nanoparticles65. Computational stud-
which include the toroidal response is still ongoing23,24,47,50,71. ies demonstrated that an inhomogeneous dielectric environment
Both charge-current multipole expansion and Mie theory provide Correspondingly, Mie expansion features scattering contribu-
a complete mathematical description of electromagnetic scatter- tions of only two kinds, as defined by the resulting two sets of Mie
ing in the far field. However, toroidal excitations appear only in the scattering coefficients al,m and bl,m (ref. 90):
multipole expansion explicitly and in the Mie expansion inexplicitly,
as explained below.
Esca= k2 Σ (A
l,m
a Ψ + Bl,mbl,mΦl,m)
l,m l,m l,m
perturbs the non-radiating charge-current configuration leading to not only the fields but also the associated potentials are unobservable
directional emission75. everywhere exterior to the spatially localized non-radiating source,
It was suggested that, non-radiating configurations composed of while Aharonov-Bohm-type effects associated with non-radiating
electric and toroidal dipoles act as sources of propagating electro- potentials are only possible in static situations76.
magnetic potentials14 (Fig. 4), that can be used as a new channel for Recently, the weak interaction of non-radiating configurations
information transfer in time-dependent Aharonov-Bohm-like exper- and static toroidal moments with electromagnetic fields has been
iments. These suggestions were later challenged; it was argued that discussed as a barrier that can protect superconducting qubits from
a b c
d e f
2.4 eV 2.8 eV
2.5 eV 3 eV
g h i
Figure 3 | Toroidal metamaterials. a, Artistic drawing of the metamaterial unit cell used for the first demonstration of a dynamic toroidal dipole absorption
resonance51. b, A planar low-loss split-ring metamaterial on a dielectric substrate supports toroidal modes of excitation57. c, A scaled-down version of
the metamaterial presented in a shows plasmonic toroidal response at optical wavelengths61. d, An optical toroidal metamaterial exploiting resonant
plasmonic response62. e, A spoof plasmon structure supports a toroidal dipole excitation at oblique angles of incidence67. f, Plasmonic oligomers consisting
of voids in metallic films exhibit toroidal response at visible wavelengths and can be excited by a free-electron beam68. g, Low-loss toroidal metamaterial
consisting of dielectric cylinders70. h, Interference of induced electric and toroidal dipoles in a resonantly transparent metamaterial consisting of
dumbbell-shaped apertures leads to a non-radiating configuration73. i, Near-field signature of toroidal dipole excitation in a dielectric nanoparticle48. Figure
reproduced from: b, ref. 57, APS; d, ref. 62, AIP; e, ref. 67, OSA; f, ref. 68, American Chemical Society; i, ref. 48, NPG.
environmental disturbances77. In the past, optical activity, a phe- lemmas, provided that the space- and time-dependencies of the
nomenon of polarization rotation of electromagnetic waves travel- two sources cannot be separated or that they do not share the same
ling through chiral media, was linked to the presence of the electric form of time dependence10. This was illustrated by the interactions
and magnetic dipole (or electric quadrupole) moments1. It is now between currents in a toroidal coil and in a ring with different time
understood that combinations of electric and magnetic moments dependence, that allegedly breaks action–reaction equality. We are
with toroidal moments can also give rise to optical activity54. A not aware of any independent verification of this result.
recent experimental demonstration showed a dominant role for
the toroidal moment in the polarization properties of a purposely Propagating toroidal excitations
designed microwave metamaterial78. Although most works on toroidal electrodynamics were focused on
Finally, it has been argued that electrodynamic interactions the localized toroidal excitations of matter, a new form of free-space
between toroidal sources, and electric or magnetic sources could vio- propagating toroidal excitation was predicted79 in 1996 and has
late the standard (Lorentz and Feld-Tai) formulation of reciprocity recently begun to receive attention80,81. Known as ‘focused doughnuts’,
q2
Vanishing fields
Vanishing fields
q1
H
Propaga
ting potentials