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PHOTONICS Research

Twisted light and twisted matter: the photonic frontier of chirality [Invited]
Kayn A. Forbes®
School of Chemistry, University of East Anglia, Norwich NR4 7TJ, UK (k.forbes@uea.ac.uk)
Received 31 July 2025; revised 18 September 2025; accepted 25 September 2025; posted 25 September 2025 (Doc. ID 574843); published 24 December 2025
Chirality, the inability of an object to match its mirror image, is central to the architecture of life. It critically influences pharmaceuticals, catalysis, and emerging photonic technologies, where controlling handedness determines function and performance. While optical chirality has traditionally been associated with circular polarization, the advent of structured light has introduced new forms of chirality through the helical wavefronts of vortex beams carrying orbital angular momentum. These developments challenge conventional frameworks and have opened new directions in the study of chiral light-matter interactions. This review focuses on the role of wavefront chirality in two emerging areas: enhancing chiroptical spectroscopies and inducing chiral structure formation in materials. We highlight how recent advances in theory and experiment have enabled structured light to serve not only as probes of chirality but also as active agents in its generation and control. By uniting progress in theory, experiment, and application, this review positions the chirality of structured light as a transformative tool in the ongoing exploration of optical and material asymmetries. © 2026 Chinese Laser Press
https://doi.org/10.1364/PRJ.574843

1.		INTRODUCTION
Chirality, the property of an object that cannot be superimposed on its mirror image, is a fundamental feature of nature, permeating chemistry, biology, physics, and materials science. It underpins the very fabric of life: protein-building amino acids are exclusively left-handed, while most biologically relevant sugars are right-handed. This molecular handedness is not incidental—it reflects the exquisite selectivity and efficiency of biological processes. Given the constraints of biochemical complexity and energy optimization, it is plausible that life elsewhere in the universe would also exhibit molecular chirality [1]. Beyond biology, chirality plays a critical role in pharmaceuticals [2], catalysis [3], and optical sensing and spectroscopy [4,5], where the ability to distinguish between enantiomers is essential both for practical applications and for advancing fundamental science.
In recent years, photonics has emerged as a uniquely powerful platform for exploring and manipulating chirality. For over a century, optical chirality research has primarily centered on molecular systems probed by circularly polarized plane waves [6]. However, the advent of nanophotonics, and with it, the ability to sculpt matter in three dimensions at the nanoscale, has propelled chiral materials science into a new era [7-9]. Advances in plasmonic [10] and all-dielectric metastructures now enable tailored chiroptical responses far beyond those achievable with natural molecules. Simultaneously, the emergence of structured light [11,12] has introduced entirely novel
2327-9125/26/01B193-16 Journal © 2026 Chinese Laser Press optical geometries, including optical vortex beams with helical wavefronts conveying orbital angular momentum [13], offering chiral degrees of freedom that are independent of polarization helicity. These advances challenge the traditional association of optical chirality with circular polarization alone, expanding the toolkit for both fundamental investigations and applied technologies. In this way, light has become not just a probe of chirality, but a tool for its generation, modulation, and control.
This review surveys a frontier of chiral photonics that exploits the wavefront chirality of twisted light beams in two distinct ways: to develop new chiroptical techniques for probing chiral matter with greater sensitivity, and to actively induce novel forms of twisted matter. While prior reviews have addressed optical chirality broadly, our focus is on wavefront chirality and its dual roles in probing and shaping chiral systems. We begin with brief foundational overviews of asymmetry in light and matter (Section 2) and chiral light-matter interactions (Section 3). The core of the article examines optical activity with structured light (Section 4) and the use of twisted beams to generate chiral nanostructures (Section 5). We conclude with a summary and discussion of future directions.
2.		HANDED UNIVERSE: CHIRALITY IN LIGHT AND MATTER
The concept of chirality is often first encountered in material objects such as our hands or chiral molecules. In group theory, an object is chiral if it lacks all improper symmetry operations—
Corrected 21 January 2026

namely, a center of inversion, mirror planes, or rotation-reflection axes. As such, it must belong to one of the chiral point groups: C„, Dn, O, T, or I.
Even more profound than spatial symmetries is the fact that symmetry is embedded in the fundamental laws of physics themselves. This is embodied in CPT symmetry, which combines charge conjugation (C), parity inversion (P), and time reversal (Τ). Charge conjugation arises from relativistic quantum field theory and plays little role in optics. However, the behavior of physical quantities under Ρ and Τ is directly connected to chirality [6,14,15]. This leads to the distinction between scalars, pseudoscalars, vectors, and pseudovectors.
•		Pseudoscalars change sign under parity but behave like scalars under proper rotations. Their behavior under time reversal depends on what they are built from: many classical examples (e.g., optical chirality) are time-even, but in general they need not be.
•		Pseudovectors (axial vectors) are invariant under parity transformations, whereas true vectors change sign. As with pseudoscalars, their time-reversal properties depend on the underlying quantities (angular momentum and magnetic fields are time-odd, but this is not universal).
This classification has important implications. The concept of true chirality, introduced by Barron [16,17], refers to dissymmetries that are space-odd and time-even, i.e., described by pseudoscalar observables. Other dissymmetries, such as space-even, time-odd quantities, are considered false chirality. This distinction will prove crucial throughout this review, as many observables in modern chiral photonics exhibit one or the other. This also reinforces the fact that optical helicity— or optical chirality—a pseudoscalar quantity, should not be used synonymously with spin angular momentum, which is a pseudovector, in the most general case [18,19], even though the two are directly proportional in the paraxial regime (see Box 1).
True chiral observables include natural optical rotation, circular dichroism, and related effects—all of which are associated with pseudoscalar quantities, such as the optical rotatory strength. Pseudovector observables, on the other hand, under-

Box 1. Optical properties of paraxial vortex beams

= — Im(E* · VE) =
2ω7

hkì.

Energy density The time-averaged energy density u of a paraxial Laguerre—Gaussian (LG) beam is proportional to its intensity ILG> with the field profile given by the well-known mode VI [20]:
u = $ |E|2 ==wfar2 = ^ perphoton: Avon.

The ring radius increases with C and the radial number produces p + 1 rings of intensity.
Canonical (orbital) momentum density The canonical (or orbital) momentum density for a z-propagating LG beam is given by
ILG(- 2\
	I k2 		φ perphoton
cw r
Helicity density For monochromatic beams, the helicity density is proportional to the optical chirality density C [21] and reflects the degree of ellipticity in the paraxial polarization. It reaches its maximum magnitude for circular polarization, where σ = ±1 denotes left- or right-handedness:
Co	C
h = —— Im(E* - B) = o— = = > perphoton:	oh.
2ω V 7	020 0211

Poynting momentum density Using purely transverse (paraxial) fields leads to the Poynting momentum density being purely longitudinal (in contrast to the canonical momentum density). To highlight the important azimuthal components requires inclusion of the non-paraxial longitudinal fields [see Eqs. (8) and (9)] and gives at z = 0

x [um]	x[um]

Note that in the case of o = 0, the canonical and Poynting momenta coincide.

e0 Τ	P ILG 1	. X
s = — lm(E x E) = σ	z perphoton. OhL.
20	εω

ILG,,9.	A
1 = r x p = 	(-kró + ^ζ) perphoton: fhz. CO

Spin angular momentum density The spin angular momentum density of a paraxial beam is equivalent to the helicity density directed along the propagation axis:
Orbital angular momentum density The /-dependent orbital angular momentum density is directed along the propagation axis and its spatial distribution matches the beam intensity profile:

Fig. 1. Chiral objects cannot be superimposed on their mirror images. Snail shells are chiral, with right-handedness (R) being almost universal across species. A left-circularly polarized wave 6 = 1 flips helicity upon reflection, becoming a right-handed wave σ = -1. Similarly, a left-handed wavefront / = 1 transforms into a righthanded one / = -1 under parity. While σ and € themselves are pseudoscalars and change sign under reflection, the corresponding spin and orbital angular momentum-σnk and /hk per photon-are pseudovectors and remain unchanged. This is because the direction of propagation k also inverts, rendering the total angular momentum vectors even under parity.

pin phenomena like magnetic optical activity. It is also important to stress that while the light or the molecule alone may break Ρ or Τ, the total light—matter system in any measurable optical process always respects both Ρ and Τ symmetry.
Historically, chirality in light was primarily associated with its polarization. Circularly polarized light traces a helical path as it propagates, twisting either left or right. This handedness is described by the pseudoscalar helicity 6: 6 = +1 for lefthanded circular polarization, o = -1 for right-handed, and σ = 0 for linearly polarized or unpolarized light (Fig. 1). Elliptically polarized light lies between these extremes and carries a reduced helicity o| < 1, still retaining a handedness. The helicity thus encodes geometric chirality in the polarization state.
More recently, attention has turned to chirality embedded in the phase structure of light. Twisted light, such as Laguerre- Gaussian beams, possesses an azimuthally varying phase of the form
exp(it),
where € € Z is the topological charge and φ is the azimuthal angle. This phase structure results in a helicoidal wavefront: / > 0 corresponds to a left-handed twist, and / < 0 to right-handed (Fig. 1). As such, the pseudoscalar € serves a role in wavefront chirality analogous to that of o in polarization chirality This review focuses on how the pseudocscalar € of twisted light can be harnessed in two distinct ways: first, to passively probe and characterize chiral materials via optical activity; and second, to actively generate novel twisted nanostructures and metamaterials.
3.		OPTICAL FORCES AND CHIRAL LIGHTMATTER INTERACTIONS WITH TWISTED LIGHT
Among the various formalisms used to describe light-matter interactions, the multipolar interaction Hamiltonian stands out as particularly effective. Applicable in both semi-classical and fully quantum formulations [6,22,23]-where it is known as the Power-Zienau-Woolley (PZW) Hamiltonian in the lat- ter-it proves especially valuable for analyzing chiral lightmatter interactions. By including the first-order magnetic dipole and electric quadrupole corrections to the dominant electric dipole term, the interaction Hamiltonian takes the form
Hint = -p-E-m-B-Q„V,E,+ .... (1)
Here,μ, m, and Qij denote the electric dipole, magnetic dipole, and electric quadrupole moments, respectively, while Ε and Β are the electric and magnetic fields. The first term in Eq. (1) corresponds to the well-known electric dipole (El) interaction, which dominates most light—matter processes. For a given optical interaction, a quantum amplitude (or matrix element) is constructed as a linear combination of such El terms—e.g., single-photon absorption involves a single E1 interaction. The corresponding observable rate is then obtained via Fermi’s golden rule, involving the modulus squared of the amplitude [24].
When higher-order terms such as the magnetic dipole (Ml) and electric quadrupole (Ε2) are included, interference between El and Ml or El and E2 terms in the rate gives rise to natural optical activity [6,22]. Similarly, false chirality can be described by incorporating static coupling terms into the Hamiltonian. In such cases, it is again the interference effects that give rise to phenomena such as magnetic and magneto-chiral optical activity.
For purely dipolar interactions, chiral light—matter coupling and optical forces can be compactly described using dipolar polarizabilities and well-established quadratic field quantities [25,26]. The temporally and rotationally averaged absorption rate A for an isotropic electric dipole—equally applicable to gases and liquid solutions-is expressed in terms of the electric polarizability a and the electromagnetic energy density u. In contrast, the dipolar chiral absorption rate Achiral, solely responsible for circular dichroism in solutions for example, involves the mixed electric-magnetic polarizability tensor Xij> whose isotropic part is defined as > = ITrxij and is proportional to the optical helicity density h, directly proportional to the optical chirality density C for monochromatic beams [27-29] (using electrodynamic units c == €0 = P0 = 1):
A = 2@ Im[a]u, (2)
Achiral = -2a2 Imlz]. (3)
The usual electric dipole contributions to the optical gradient and radiation pressure forces are proportional to the gradient of the energy density u and the canonical momentum density p, respectively (not the kinetic Poynting momentum

Π) [25]. The chiral optical force responsible for enantioselective tweezing corresponds to the gradient of the optical helicity h [27], while the radiation pressure force involves a combination of the spin angular momentum density s [in Eq. (5) the dual- symmetric [32] form that includes the contribution from the magnetic field should be used] and the curl of the Poynting vector Π:
F = Re[a]Vu + 20 Im[a]p, (4)
Faial = -@Re[x]Vb+Imz (-26 s+V *II). (5)
Chiral optical torque, meanwhile, is proportional to the Poynting vector itself whereas the electric-dipole torque is generated by the spin s:
T = 2w Im[a]s, (6)
Tehimi = -2 Im[z]T (7)
The reader is invited to look at Box 1 at this stage to get an appreciation for the spatial distribution of various optical properties involved in Eqs. (2)—(7) and how they influence the absorption, forces, and torques.
Beyond the dipolar regime, the inclusion of electric quadrupole and higher-order multipole contributions (alongside selfinteraction) leads to a significantly more complex picture, in which the simple correspondence between response functions and local field quantities generally breaks down [31,32]. This breakdown is well-documented for large structures [33], such as Mie-resonant particles [34], but it applies equally to chiral molecules [6,35]. Moreover, beyond the relatively simple lightmatter interactions described by Eqs. (2)-(7), there exists a rich landscape of additional mechanisms, including optical rotation, Rayleigh and Raman optical activity, as well as a broad array of nonlinear chiroptical techniques [6,22,36,37].
By structuring and twisting light, we manipulate the electromagnetic fields E and B, thereby directly shaping field-derived quantities such as the optical helicity (chirality) density h, spin angular momentum density s, kinetic momentum density Π, and the field gradient tensor VE. Conversely, by structuring and twisting matter, we can elicit novel material responses through tailored electric dipole μ, magnetic dipole m, electric quadrupole Q^, and mixed electric—magnetic %-type moments. Acting independently or in concert, twisted light and twisted matter are opening new frontiers in light—matter interaction. In the following sections, we carry out the main aim of our review and survey recent efforts toward this rapidly evolving goal.
4.		OPTICAL ACTIVITY DRIVEN BY STRUCTURED AND COMPLEX FIELDS
In this section we survey studies that tailor the electromagnetic fields E and Β with the aim of driving novel forms of optical activity. In particular, we are predominantly interested in chiral light—matter interactions involving twisted beams, where E and B carry the azimuthal phase structure exp(ie p), producing a chiral helical wavefront. As an example of the type of question we seek to answer: just as the pseudoscalar helicity σ of circularly polarized light gives rise to natural circular dichroism (CD), can the orbital angular momentum pseudoscalar € similarly give rise to an analogous effect known as vortex dichroism (VD)? This effect is also referred to in the literature as helical dichroism (HD) or orbital dichroism (OD)-here we adopt the convention that “dichroism” refers specifically to resonant absorption, distinguishing it from differential scattering. Since polarization and phase are independent degrees of freedom, we further investigate the combined influence of circular polarization and optical vortices through what we term circular vortex dichroism (CVD).
The corresponding differential intensity I contrasts, which we aim to experimentally measure, can be defined as

CVD

To=1 To=-1
777=1 I To=-1' 1 ±| | T I
Here, CD quantifies the differential response to left- and right-handed circularly polarized light, independent of €. VD quantifies the differential response to left- and righthanded optical vortices (positive and negative €), independent of polarization. For CVD, we distinguish two regimes:
•		parallel CVD: comparing beams with the same handedness in σ and l (e.g., both positive or both negative);
•		antiparallel CVD: comparing beams with opposite handedness in o and € (e.g., o = 1 with / = -1 versus o = -1 with € = 1).
Finally it is instructive to produce here the electric and magnetic field structures of a Laguerre—Gaussian mode in cylindrical coordinates (τ,φ,ζ), including the paraxial and non- paraxial field components; the former transverse with respect to propagation direction z, the latter longitudinal to z. Without the longitudinal component, the paraxial beams do not satisfy the Gauss’s laws V-Ε = 0 and V B = 0 [38]. For simplicity we provide the field structures for p = 0 circularly polarized LG beams at the focal plane z = 0 [39]:

x + ioy + 22

|Z|

e "e.

(8)

. , y - iox + — z
.k

Id,2.
w? ill e 000,

(9) where y(p,z = 0) = E - 2;; wo is the beam waist, and E0 is the amplitude [the most general definitions of Eqs. (8) and (9) can be found in Ref. [40]}. Note that it was the transverse (x, y) components of Eqs. (8) and (9) that calculated the optical properties in Box 1 (where the Poynting momentum required the z-components to highlight its azimuthal component). The magnitudes of the longitudinal components E2 and Bz, relative to their respective paraxial transverse components, are scaled by the so-called paraxial parameter 1/kw0, where k = 2^/2 is the wavenumber. Thus, unless W0 & 2, the longitudinal component is negligible compared to the transverse field components.
This explains why paraxial optics remains highly valuable in most applications, only breaking down under tightly focused conditions-an important regime for understanding the chirality of twisted light, as we shall see.
A.		Chiral Dipoles
The first investigation into the optical activity of structured light was conducted by Andrews et al. [41], who theoretically examined whether the helical phase front of optical vortex beams could induce an -dependent dichroism in chiral molecules, similar to the σ-dependence shown for circularly polarized light in circular dichroism. In their theory they looked at the electric dipole-magnetic dipole (E1M1) mechanism of single-photon absorption in a freely tumbling collection of chiral molecules subjected to a paraxial Laguerre-Gaussian beam and concluded there is no /-dependent chiral effect-an outcome later confirmed experimentally using Laguerre—Gaussian modes [42].
As in conventional linear optical activity, circular dichroism in chiral solutions arises from E1M1 interference and is proportional to the optical chirality density C [see Eq. (3) and Box 1]- note we use optical chirality rather than optical helicity from now on to coincide with the quantity most used in the literature. However, in the paraxial limit—neglecting the longitudinal fields in Eqs. (8) and (9)-C remains insensitive to the wavefront chirality. This is because, in the transverse electric and magnetic fields, only the phase terms exp(ilp) carry a linear dependence on l, and their product in C x Im(E* · Β) trivially evaluates to unity.
This finding highlights the scale mismatch between the global phase structure of vortex beams and the localized, molecular-scale chirality of typical matter systems. Circular polarization, as a local property, traces a helical trajectory with spatial extent on the order of the optical wavelength, enabling weak but non-negligible coupling to nanoscale chiral dipoles. In contrast, the helical wavefront associated with orbital angular momentum spans the entire beam waist and for collimated or weakly focused beams, w > 2, the resulting spatial overlap with chiral dipoles is extremely poor—rendering wavefront chirality largely ineffective in such regimes. However, under tight focusing, the beam waist contracts to near-wavelength dimensions, and significant longitudinal field components emerge that explicitly carry a linear dependence on € [Eqs. (8) and (9)]. These non- paraxial fields introduce new /-dependent contributions to the optical chirality density C, including terms that arise from the longitudinal and higher-order transverse modes in the electric and magnetic fields [40,43,44]. The optical chirality density for tightly focused Laguerre-Gaussian modes, first derived in Refs. [43,44], can be written using Eqs. (5) and (6) as
c-+f(P +S)-3] 00

Fig. 2. Optical chirality densities of focused Laguerre—Gaussian beams (compared to Box 1 for paraxial LG beams), (a) Polarization-independent contribution to the optical chirality density of LG beams, relevant for unpolarized and linearly polarized input modes. This contribution originates purely from the longitudinal field components and locally reverses sign with a change in the handedness of l. (b) Optical chirality density of a circularly polarized LG beam. The first column shows the contribution from the transverse fields, the middle from the longitudinal fields, and the final column presents their sum. Spin-orbit interactions result in a non-zero on-axis chirality density when the signs of € and σ are opposite. Reproduced with permission from Ref. [44],

The first term in square brackets corresponds to the well- known optical chirality density of a circularly polarized paraxial beam (Box 1). Its pseudoscalar-dependence stems purely from the helicity σ and is proportional to the beam intensity and the polarization handedness. The remaining σ-dependent terms represent non-paraxial corrections to the paraxial optical chirality density, and each possesses a distinct spatial distribution. As we will see, these terms give rise to novel spin—orbit interactions in the optical chirality field. The final term is of particular interest:

it is linearly dependent on the topological charge € and independent of σ. This contribution arises purely from the longitudinal field component E*Bz, and under tight focusing, it enables wavefront chirality-previously ineffective in paraxial regimes-to engage in chiral light-matter interactions. Notably, although this term does not contribute to the integrated optical chirality, it generates a spatially structured C distribution (Fig. 2) that may locally enhance chiral sensitivity. The spatial distribution of Eq. (10) for various input values of € and o are presented in Fig. 2.
The first study to highlight the significance of the longitudinal fields of vortex modes in chiral interactions investigated a co-propagating, coherent superposition of / = ±1 linearly polarized (σ = 0) Bessel beams [45]. The authors demonstrated theoretically that at the beam center (r = 0), where only longitudinal electromagnetic fields are present, local enhancements of the optical chirality density C can exceed those achievable using circular polarization alone.
The first experimental observation of /-dependent optical activity in chiral dipoles was reported by Wozniak et al.
[46], who focused linearly polarized Laguerre-Gaussian beams onto individual right- and left-handed nanoscale chiral gold helices and observed a differential transmission between / = +1 and / = -1 beams, i.e., vortex dichroism, as exhibited in Fig. 3(a). By positioning the nanostructure at the beam center, the electric-magnetic dipole (E1M1) interaction enabled coupling to the optical chirality density C via Eq. (3), resulting in the right-handed helix coupling more strongly to / = -1 and the left-handed helix to / = +1.
Wu et al. [47] numerically demonstrated that a chiral molecule positioned between plasmonic nanoparticles exhibits a strong vortex dichroism signal proportional to Eq. (10) (when o = 0), even when the nanoparticles themselves are achiral. The chiroptical signal increases with the sign of € and survives orientational averaging of the particles.

Fig . 3. (a) Vortex dichroism in a chiral gold nanohelix positioned at the center of the optical chirality density of focused / = ±1 linearly polarized Laguerre—Gaussian beams. The right-handed nanostructure absorbs / = -1 beams less than 2 = +1, generating a differential transmission signal, (b) Vortex dichroism measured using an X-ray beamline source. A spiral Fresnel zone plate is used to generate and focus / = ±1 and l = ±3 vortex beams onto a powder sample of a chiral organometallic complex. Above approximately 7120 eV, strong and distinct dichroism is observed that depends on the sign of ^. (a) Reproduced with permission from Ref. [46]; (b) from Ref. [48].

Rouxel et al. [48] measured vortex dichroism in enantiopure powders of chiral organometallic complexes using linearly polarized hard X-rays shaped and tightly focused by spiral Fresnel zone plates, achieving asymmetry ratios up to 5%,

vastly exceeding those in comparable CD experiments [Fig. 3(b)].
The studies mentioned so far have been concerned with linearly polarized vortex beams σ = 0, f # 0. By employing linearly polarized light, any contribution from polarization chirality σ was eliminated, ensuring that the observed and predicted dichroism originated solely from wavefront chirality €, described by the final term in square brackets of Eq. (10). A broad basis for chiral effects with vortex beams was developed by Forbes and Jones [49], who identified the four forms of dichroism in vortex beams arising from combinations of o and €: CD, VD, and two types of CVD. The spatial profile of C and the corresponding dichroism rate strongly depend on whether € and σ are parallel (same sign) or antiparallel (opposite sign)- akin to spin-orbit coupling effects observed in the intensity patterns of tightly focused optical vortices [50,51]. In particular, for parallel combinations sgn l = sgn σ the spatial distribution of CVD is identically zero on-axis; for anti-parallel combinations sgn € = -sgn σ there is an on-axis chirality density for values of |/| = 1, 2 [52,53] [Fig. 2(b)], and the rate of CVD has been shown to exceed that of CD.
A key insight from Eq. (10) is that the ^-dependent term remains even after averaging over both orthogonal polarizations (σ = ±1), meaning optical chirality can arise from unpolarized vortex beams [54], and that remarkably unpolarized light can produce chiral light-matter interactions. This unexpected result has been explored in several follow-up studies [44,52], which showed that the spatial distribution and magnitude of C can be tuned via C, beam ellipticity, degree of polarization, radial index p, and focusing strength. Notably, unpolarized vortex beams can even generate enantioselective tweezing forces via the first term in Eq. (5), enabling all-optical separation of chiral particles [55]. Enantioselective forces dependent on both the topological charge and polarization state of vortex beams have been reported to exceed those of conventional optical-forcebased chiral resolution methods by up to two orders of magnitude [56].
The majority of studies, including all discussed so far, have been in the linear optics regime. However, the nonlinear optics of structured light is rapidly gaining recognition as an exceptionally rich area of study where the true advantages of complex beams emerge [11]. There have been a few promising investigations into the nonlinear optical activity of structured light: Mayer et al. [57] demonstrated enantiosensitive high-harmonic generation using synthetic chiral light composed of vortex beams, and Cheeseman and Forbes [58] reported nonlinear vortex dichroism in two-photon absorption, which exhibited a pronounced dependence on the orientation of the linear polarization, as well as novel selection rules that enable probing of otherwise inaccessible molecular features.
Shi et al. [59] theoretically investigated the generation of optical chirality in photonic jets formed by high-index dielectric microspheres illuminated with LG beams. Acting as microlenses, the microspheres produce tightly confined, high-intensity near-fìeld regions, known as photonic jets, just beyond the shadow-side surface. These jets, with field distributions highly sensitive to the size, refractive index, and structural properties of the particle, can be engineered to produce enhanced and spatially localized optical chirality. Building on this concept, Shi et al. [60] extended the idea to Janus particles composed of two hemispheres with different refractive indices. These asymmetrical spheres break the axial symmetry of the jet and give rise to photonic hooks-curved light beams that deviate from the typical linear photonic jet trajectory. The study demonstrated that the optical chirality distribution induced by vortex beams in such systems also follows this curvature, resulting in spatially displaced and directionally bent chiral hotspots. Together, these studies reveal that both conventional and curved photonic near-fìeld structures can serve as powerful tools for engineering local chirality of vortex beams at the subwavelength scale.
Vector beams with inhomogeneous polarization distributions nominally possess zero optical chirality density C, as is the case for radial and azimuthal vector modes, corresponding to transverse magnetic (TM) and transverse electric (ΤΕ) modes, respectively. Herrero-Parareda and Capolino [61] demonstrated that when these modes are coherently superposed into a spirally polarized beam, a non-zero C emerges due to the generation of longitudinal field components. In a more general analysis, Forbes [62] showed that higher-order and hybridorder vector vortex beams exhibit intricate field structures that give rise to highly patterned C distributions, which are closely linked to their Pancharatnam topological charge. It is important to note, however, that the optical chirality of vector vortex beams cannot exceed that of scalar vortex beams [63,64]. Liu et al. [65] measured enantiomeric excess with micrometer precision by spatially resolving the local polarization angles of radial vector beams after undergoing optical rotation in chiral solutions.
B.		Chiral Interactions beyond the Dipole
Beyond electric and magnetic dipole interactions, structured light offers significant opportunities for driving novel lightmatter interactions. Higher-order multipoles, such as electric quadrupoles, couple to field gradients, which in structured beams can be far richer and more intense than in conventional Gaussian beams. For example, in the interaction Hamiltonian, Eq. (1), the electric quadrupole term couples directly to the electric field gradient:

/ i ( Co ( , Co Co
+ (	7 	e"7*' Fy +y - γ 	Η—
X r ) XX	r r-)
i(e+o),YYEp 44
+ 	Φ + ikz ) ) VLG	(11)
where we used Eq. (8) for E; and VIA is the well-known mode amplitude for LG beams [20]. In comparison, if the beam were a simple paraxial Gaussian, only the r- and /-dependent terms in the first line of Eq. (11) would contribute appreciably. The additional transverse and azimuthal gradients arising from beam structure—e.g., the € - and σ-dependent terms—vanish in the absence of twist, thereby suppressing the coupling to higher multipoles. Beyond molecular matter, higher-order multipoles also play a central role in many plasmonic nanostructures, where intense near-fìeld gradients and strong field

confinement readily excite quadrupole, octupole, and even higher-order modes [66,67]. These contributions are especially pronounced in chiral or anisotropic geometries, where symmetry breaking permits non-dipolar channels to dominate the optical response—particularly under structured illumination.
The first study to highlight the potential importance of electric quadrupoles in chiral twisted light-matter interactions appeared in 2016. Brullot et al. [68] observed differential transmission of linearly polarized vortex beams through nanoparticle-bound phenylalanine enantiomers, which they attributed to electric quadrupolar coupling of the form Q„V;E). This vortex dichroism enabled enantiomers to be resolved at wavelengths far from their circular dichroism resonances, with observed VD differentials reaching up to 0.6%-significantly larger than typical CD signals, which are generally in the range of 0.01%-0.1%.
A firmer theoretical foundation was established by Forbes and Andrews [69], who demonstrated that, even within the paraxial regime, the azimuthal field gradient introduces ^-dependent quadrupolar contributions via the Ε1Ε2 interaction mechanism. Quadrupole effects have since been explored in various chiroptical phenomena, including Raman optical activity [70,71], and hyper-Rayleigh and hyper-Raman scattering [72]. In contrast to dichroic (absorption) effects, the Ε2 contributions to scattering mechanisms of optical activity persist under orientational averaging. Notably, for similar reasons outlined in chiral dipoles (they depend on transverse structure), /-dependent Ε2 interactions become significantly enhanced under tight focusing, where longitudinal field gradients can rival those of the transverse field in paraxial beams.

Fig. 4. (a) Gigantic vortex differential scattering of linearly polarized vortex beams by chiral microstructures reveals the scale-dependent nature of chirality. Increasing the value of € increases the ring radius of vortex modes: at low and high values of ^ the vortex beam is much smaller or larger, respectively, than the chiral structure, leading to weak spatial overlap. For values around € = 30-40, strong spatial overlap occurs and large differential scattering between / > 0 and / < 0 beams is observed, (b) By adsorbing chiral molecules onto a chiral microstructure, the combination of vortex chirality and plasmonic enhancement leads to gigantic vortex differential signals, enabling enantiomer identification, (c) Significant vortex dichroism in metallic propeller metastructures is observed, generated through magnetic quadrupole couplings, (a), (b) Reproduced with permission from Ref. [73]; (c) from Ref. [75].

For reasons opposite to those underlying the very weak C- dependent chiroptical signals produced in chiral dipoles by paraxial vortex beams, artificially designed chiral microstructures typically also exhibit only weak responses to circularly polarized light. The experiments by Ni ci al. [73] provide a striking demonstration of the scale-dependent nature of vortex wavefront chirality and its practical advantages for chiroptical detection in large structures. Using chiral microstructures, they observed gigantic vortex differential scattering-up to 120% contrast between |2| and -|2|-for linearly polarized beams [Fig. 4(a)]. Crucially, they showed that this effect is maximized when the beam width is matched to the lateral size of the chiral microstructure. This was achieved by controlling the radius of the vortex intensity ring, re = woVII/2, and second moment

radius W2 = woVI+1 through variation of the topological charge € [74]. In the same study, highlighted in Fig. 4(b), the authors also demonstrated femtomole-level enantioselective sensitivity for phenylalanine enantiomers, enabled by a plasmon-enhanced (25%) vortex differential scattering mechanism—a significant improvement over conventional circular differential scattering techniques. The same group has conducted several follow-up studies exploring vortex differential scattering in a range of chiral nanostructures. These include the observation of a magnetic quadrupole-induced vortex dichroism mechanism in metallic propeller meta-molecules [Fig. 4(c)] [75]; a vortex differential scattering of approximately 23% in three-dimensional chiral oligomers [76]; around 50% in chiral copper microhelices [77]; about 20% in planar chiral nanostructures [78]; ~100% in stereometamaterials [79]; and up to 75% in a tunable chiral metamaterial where the handedness can be reversibly switched by applying a static external magnetic field [80]. In contrast to the differential vortex scattering mechanisms described above, Wang et al. [81] observed a resonant differential effect (vortex dichroism) in twisted dielectric metastructures using strongly focused vortex beams.
Other studies on plasmonic systems include using a chiral metamaterial structure composed of two elliptical silica rods covered with a gold film on a substrate to achieve a vortex dichroism of up to 58.5% [82]. Lim et al. [83] experimentally observed large vortex dichroism in an array of 3D chiral plasmonic gold helicoid III structures. Using multipolar simulations the underlying mechanism was determined to be an interference between electric and magnetic quadrupole moments. Kerber et al. [84] numerically investigated four classes of differential scattering of circularly polarized vortex beams in plasmonic nanoantenna monomers, dimers, and trimers. While monomers show only standard circular dichroism, dimers and trimers exhibit /-dependent scattering, with trimers able to distinguish the sign of l, an effect with a magnitude comparable to normal circular dichroism. While no multipolar analysis was undertaken, the observed effects depend on spin—orbit interaction, helicity, and the angular arrangement of nanoantennas, becoming achiral at specific orientations. Simulations by Reddy et al. [85] show that circularly polarized Laguerre- Gaussian beams strongly enhance chiral responses in plasmonic metasurfaces of gold nanohelices, with OAM-assisted circular dichroism (CVD) up to 200x stronger than conventional CD. The dichroic signal flips sign with opposite l and scales with helix spacing, likely due to enhanced quadrupole interactions transferring OAM to surface electron oscillations. Lalaguna et al. [86] exploited the SAM and OAM of focused Laguerre—Gaussian modes to actively modulate optical activity in chiral metasurfaces, demonstrating that the presence of OAM enables excitation of otherwise dark modes.
Beyond plasmonic structures, Wang et al. [87] theoretically studied vortex differential scattering in dielectric chiral particles. Their simulations showed the differential scattering could be enhanced by increasing the chirality parameter of the material, tight focusing, inclusion of circularly polarized light, and using non-spherical particles. The Bhardwaj group has undertaken a number of studies looking at a non-resonant, nonlinear form of /-dependent light-matter interactions in chiral molecular solutions [88,89] and solids [90]. Mùllner et al. [91] studied how vortex light interacts with chiral liquid crystals using Raman scattering, showing that both σ and € can engage with the material’s chiral structure. They identified two distinct signals: a higher-energy component with helical polarization linked to SAM, and a lower-energy, broader signal associated with OAM transfer.
Terahertz optical vortices have been shown to interact with magnetized dysprosium iron garnet in a dichroic manner, with the response governed jointly by the vortex’s topological charge and an externally induced magnetization from neodymium magnets [92]. Fanciulli et al. [93,94] have pioneered studies of differential reflection and transmission of optical vortices incident on magnetic vortices—microscale ferromagnetic disks where the magnetization curls in-plane around a core with out-of-plane magnetization, forming a stable swirling pattern. In their recent experimental work [94], they observed a form of magnetic vortex dichroism by measuring the resonant scattering of extreme ultraviolet light carrying orbital angular momentum from permalloy dots in a magnetic vortex state. By switching the direction of the magnetic vortex core magnetization, they detected strong dichroic asymmetries in the reflected light intensity profiles dependent on the topological charge of the incoming vortex beam. These asymmetries arise from interference between optical modes differing by one unit of OAM, directly linked to the curling magnetization of the vortex. Their results, shown in Fig. 5, demonstrate magnetic vortex dichroism as a novel optical probe for magnetic structures and topology, with potential for ultrafast studies and control of complex spin textures. These studies were recently expanded to the time-domain [96].
5.		MATERIAL SCIENCE WITH STRUCTURED LIGHT
Chiral molecules have been isolated from natural sources for centuries, with early chemists recognizing their unique optical activities [1]. The development of synthetic methodologies to selectively produce enantiomerically enriched compounds, however, represents a landmark advancement in chemistry, primarily achieved during the 20th century [97]. Chiroptical signals in molecules are generally very weak, with typical electronic circular dichroism (CD) dissymmetry factors in the region of < 10-2, and vibrational CD signals often on the order of 10-4 [98]. As discussed in the previous section, twisting light is one pathway to increasing this dissymmetry. Another involves the fabrication of chiral metamaterials and nanostructures, particularly those constructed from metals to exploit plasmonic field enhancement [10,95,99,100].
A wide array of fabrication strategies have been developed to construct these structures, including various forms of lithography, laser writing, colloidal synthesis, and DNA-directed assembly [10,95]. In the last decade, a completely novel approach has emerged: the use of optical vortex beams to impart twist and angular momentum directly into bulk matter, leading to the formation of chiral helical nano- and microstructures [101,102]. The idea in general consists of exposing the material to a focused optical vortex mode (usually pulsed), causing a localized solid-to-liquid phase transition and twist to the tem-
Fig. 5. Vortex dichroism in magnetic vortices. Resonant scattering of extreme UY vortex light from a magnetic vortex state leads to strong dichroic asymmetries in the reflected light intensity profiles. The differential signal can be generated by changing the sign of € or switching the curling direction of the magnetization. Reproduced with permission from Ref. [94].

Fig. 6. (a) Side view of a chiral metal nanoneedle fabricated with a Jz = 2 beam, (b) Using different combinations of spin (S2) and orbital (L2) angular momentum to form chiral nanoneedles. The twist direction of the structure is determined solely by the wavefront handedness Λ (a) Reproduced with permission from Ref. [103]; (b) from Ref. [104].

structure formation via /-dependent spiral-shaped intensity patterns (Fig. 7). These were generated either through interference between the incident OAM beam and a reflected,

porarily melted material. Once the light is switched off, the melted section resolidifies, rendering the surface with a helical morphology. Studies have demonstrated that vortex beams can twist a range of materials, including metals, semiconductors, and polymers. Interestingly, the underlying physical mechanism is yet to be fully elucidated. One hypothesis relies on angular momentum transfer from the beam to the transiently molten matter; another is based on a unique temperature profile provided by the optical field to the material [102]. This section of the review surveys the advances that have occurred in this field in just over a decade.
A.		Metals and Semiconductors
The first demonstration of spiral mass transport driven by vortex beams was reported in 2012 by Toyoda et al. [103]. Pulsed optical vortex beams carrying orbital angular momentum / = ±1 were focused onto a tantalum metal surface, where chiral, needle-like nanostructures spontaneously formed from the transiently molten metal at the dark core of the optical vortex [Fig. 6(a)]. The structures exhibited tip curvatures below 100 nm and heights of approximately 10 pm. Remarkably, the handedness of each needle was dictated by the sign of C. Further investigations [104] explored how the total orbital angular momentum Lz, spin angular momentum S2, and total angular momentum Jz influenced the formation of these chiral features [Fig. 6(a)]. No needle was formed when Lz = 0, even if Sz # 0; the handedness was determined solely by the sign of Lz, i.e., ή the spiral density (defined as the winding number divided by the structure’s length) increased with Uzl; and degenerate values of J2 could lead to identical morphologies-for example, the same chiral structure was observed for both L = 2 and Lz = 1, S. = 1.
Seeking to harness the advantages of plasmonic nanostructures, Syubaev et al. [105-107] fabricated helical needles from bulk gold and silver. In contrast to mechanisms based on angular momentum transfer, they demonstrated chiral

Fig. 7. Chiral silver nanoneedles fabricated with vortex beams of various values of € and /-dependent spiral-shaped intensity patterns with spiral arm number N. Contrary to explanations based on optical momentum mechanisms for twisted structure formation, these results suggest that temperature-driven effects can dominate over radiation forces. Reproduced with permission from Ref. [107].

speckle-modulated zero-OAM mode [106], or by employing beams with spiral-shaped intensity distributions but zero total angular momentum, produced using a binary spiral axicon [105]. Pulsed laser ablation involves rich and complex physical dynamics; in this case, the emergence of chiral structures was attributed to thermocapillary-driven spiral mass transport, induced by intensity-dependent, spiral-shaped gradients in temperature and surface tension across the metal surface [102,105-107]. Other metals where nanotwists have been fabricated using vortex beams include copper [108] and aluminum [109].
Similar behavior has been observed in semiconductors such as silicon—a material widely used in optoelectronic and photonic applications-when exposed to pulses of twisted light. Takahashi et al. [110] showed that nanosecond optical vortex pulses produce cone-shaped monocrystalline silicon structures, while picosecond pulses yield needle-like features [111]. In both cases, the chirality of the resulting structure was governed by the sign of l. Rahimian et al. [112] demonstrated the formation of twisted cone-shaped silicon structures using single femtosecond circularly polarized vortex pulses with zero total angular momentum (€ = ±1, σ = ±1). Ablez et al. [113] did a comparative study of the microneedle structuring of Si (111) and Si(lOO) with picosecond vortex pulses, the former much more readily producing helical morphology. Syubaev et al. [114] were able to tailor the chirality of silicon microprotrusions with the spiral-shaped beams discussed previously. Interestingly they were able to characterize these chiral structures using Raman optical activity.
While a fully unified physical mechanism remains to be elucidated, it is clear that twisted light offers an inexpensive and versatile optical route for fabricating chiral nanostructures, with promising applications across optics and photonics.

Fig. 8. Spiral surface reliefs formed in azopolymers exposed to focused Laguerre-Gaussian beams with topological charge € = ±10. The direction of the twist is governed both by the handedness of € and the orientation of the incident linear polarization state (indicated by white arrow insets). Reproduced with permission from Ref. [117].

B.		Polymers
Azopolymers are light-responsive materials containing azobenzene units that undergo reversible trans-cis photoisomerization upon light exposure, enabling dynamic modulation of their optical properties [115,116]. This molecular switching can drive significant surface mass transport, allowing for the direct formation of nanoscale surface relief patterns using light alone. Their sensitivity to both light intensity and polarization makes them ideal candidates for fabricating tunable photonic structures such as gratings, lenses, and waveguides.
In parallel with the first demonstration of helically nanostructured metals using optical angular momentum (OAM) by Toyoda et al. [103], Ambrosio et al. [117] reported the inaugural evidence of OAM-induced spiral mass transport in azopolymer films. By illuminating the material with tightly focused, linearly polarized Laguerre-Gaussian-like beams, they observed the formation of chiral surface relief patterns whose handedness was dictated by the sign of the topological charge € (see Fig. 8). The underlying mechanism arises from the interference between transverse and longitudinal electric field components at focus [see Eq. (8)], which produces an azimuthally varying polarization state that is dependent on both € and the input linear polarization’s state of orientation [118]. In anisotropic, photoresponsive media such as azopolymers, this spatial modulation of polarization induces inhomogeneous light

absorption, thereby driving mass transport along chiral trajectories.
The spiral surface reliefs produced by Ambrosio et al. exhibited modest peak-to-valley depths of approximately 20 nm. Building on this, Watabe et al. [119] demonstrated that conch-shell-like surface reliefs, exceeding 1 pm in height, could be inscribed in azopolymer films using circularly polarized vortex beams. The chiral morphology of these structures was directly determined by the sign of the total angular momentum J2 = Sx + Lz. Notably, they observed that such patterns only emerged under low-order vortex illumination with Jz = ±2h; using /2 = 0 or higher-order OAM modes suppressed the formation of the conch-like features, even when Lz # 0.
Often, numerical simulations are invoked to describe complex light-matter interactions; however, these can obscure the underlying physical mechanisms, which are of greater fundamental interest. In follow-up work, Barada et al. [120] developed an analytical framework to elucidate how continuous- wave vortex beams can induce twisting in isotropic, homogeneous materials, offering deeper insight into the interplay between structured light and matter. When the orbital angular momentum € and spin angular momentum σ share the same handedness, the radial force confines material within the dark vortex core, while the azimuthal force drives orbital motion clockwise or counterclockwise depending on the sign of the total angular momentum Jz. In contrast, when € and σ have opposite handedness, a repulsive radial force inhibits confinement, and the azimuthal force reverses sign across the vortex core, disrupting smooth orbital motion.
The studies described thus far rely on the chiral wavefront of a propagating vortex beam to fabricate chiral structures. It is well known that circularly polarized light can excite suitably structured plasmonic nanostructures to generate near-fìelds carrying OAM [121]. Masuda et al. [122] exploited this by using the near-fìeld OAM of a gold-plated plasmonic structure, designed as a replica of a chiral surface relief originally inscribed in an azopolymer film using a vortex beam, to induce chiral deformation in a second azopolymer thin film. The handedness of the input circular polarization σ matched that of the resulting near-fìeld OAM l, thereby determining the handedness of the newly formed chiral surface structures.
All studies examined so far have primarily relied on singlephoton absorption mechanisms to induce chiral surface structuring. In contrast, Masuda et al. [123] reported the first demonstration of chiral surface relief formation in azopolymers via a two-photon absorption process. Using picosecond vortex pulses, their approach achieved both high longitudinal and transverse spatial resolution, while notably avoiding the formation of undesired outer ring structures typically associated with the Airy diffraction pattern in single-photon processes. Other recent advances in azopolymer systems include topological control of vortex beam intensity distributions [124,125] and the imprinting of polarization skyrmions and Hopfìons [126,127] to generate chiral nanostructures.
Most optical polymers are highly transparent in the visible range (400-700 nm), allowing tight focusing of incident light for nonlinear processes such as multiphoton absorption. This transparency is crucial for photopolymerization, where

Fig. 9. C-dependent spiral intensity patterns are used to fabricate large arrays of three-dimensional chiral microstructures in an isotropic polymer. The number of entwined twists and the handedness of the chiral micro-columns are determined by the magnitude and sign of €, respectively. Reproduced with permission from Ref. [130].

absorption occurs only at the focal point due to the intensity threshold required for simultaneous absorption of multiple photons. As a result, visible-light-transparent polymers serve as ideal media for three-dimensional micro- and nanofabrication with high spatial resolution [128,129]. Ni ^al. [130] utilized the spiral intensity patterns generated by the coaxial interference of femtosecond pulsed Laguerre-Gaussian modes with a fundamental Gaussian, as discussed earlier, to fabricate large arrays of three-dimensional chiral microstructures in an isotropic polymer (Fig. 9). The number of lobes (entwined twists) and the handedness of the resulting chiral microcolumns were determined by the magnitude and sign of the topological charge l, respectively. Lee et al. [131] employed the nonlinear self-focusing of LG beams in a UV-curable resin to photopolymerize helical microfibers, with the chirality determined by the sign of the topological charge C. For / = ±1, the resulting structure consists of a single helical fiber, whereas for ||>2, the fiber splits into € intertwined branches forming C- entwined helices. These LG-beam-fabricated fibers reached maximum lengths on the sub-millimeter scale. In follow-up work, Arita et al. [132] demonstrated that / = 1 Bessel beams can produce similar helical fibers extending over a centimeter in length. Finally, Pan et al. [133] reported a rapid and highly efficient route for fabricating arrays of 3D chiral microstructures. By combining vortex-beam two-photon polymerization with capillary-force-assisted self-assembly, they achieved discrete 3D architectures displaying strong vortex differential scattering, with magnitudes approaching 30%.
6.		CONCLUDING REMARKS
Early applications of the twisted wavefronts of vortex beams centered on optical manipulation and optomechanics, where the handedness of orbital angular momentum enabled rotational control of micro- and nano-objects [134,135]. Harnessing the chirality of vortex beams for direct engagement in chiral light—matter interactions, however, remained a longstanding goal in the field of structured light since its inception over three decades ago. This review has aimed to highlight how researchers have now overcome this hurdle through a series of ingenious advances in both theory and experiment, establishing the chirality of structured light as a frontier topic in optics, light-matter interactions, and materials science.
This review has shown that structured light offers at least three distinct advantages in chiral light-matter interactions that underpin chiroptical spectroscopies: (i) significant enhancement of chiral signals; (ii) novel mechanisms independent of polarization helicity; and (iii) access to otherwise forbidden transitions, enabling structural information to be revealed beyond the limits of plane-wave excitation. These capabilities— particularly the second-suggest that the optical chirality of vortex beams is well suited for integration into miniaturized photonic devices for chiral sensing and diagnostics. Notably, the generation of nanoscale optical vortices required for such applications is itself an active and rapidly advancing area of research [136,137].
The other major focus of this review has been on how twisted beams are revolutionizing materials science by offering an inexpensive and relatively straightforward method for fabricating chiral nano- and microstructures across a wide range of materials. From helical microneedles to spiral surface reliefs and twisted fibers, the wavefront twist of vortex beams has been shown to drive the formation of such chiral metamaterials under ambient conditions, without the need for complex fabrication environments. These structures open the door to a diverse range of applications in nanotechnology, including enhanced molecular chiral sensing, optoelectronic components, and waveguides for multiplexing systems that utilize vortex beams. Indeed, cutting-edge studies have demonstrated their potential in areas such as the spatial control of conductivity in graphene [138], the modulation of enantiomeric excess during the crystallization of chiral compounds [139], unidirectional and structured light emission [140,141], and optical encryption [142].
Whether used to study material asymmetry or to create chiral structures, vortex beams have proven to be a flexible and effective tool connecting basic optical research with practical applications. As these methods continue to advance, the ability to control and apply the chirality of light is likely to play an important role in future developments in photonics, sensing, and materials science.
Acknowledgment. The author gratefully acknowledges Professor David L. Andrews for his invaluable availability and insightful discussions on symmetry.
Disclosures. The author declares no conflicts of interest.
Data Availability. No data were generated or analyzed in the presented research.
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