The question of how the orbital angular momentum of structured light might engage with chiral matter is a topic of resurgent interest. By taking account of electric quadrupole transition moments, it is shown that the handedness of the beam can indeed be exhibited in local chiral effects, being dependent on the sign of the topological charge. In the specific case of absorption, a significant interplay of wavefront structure and polarization is resolved, and clear differences in behavior are identified for systems possessing a degree of orientational order and for those that are randomly oriented.

Optical activity is conventionally understood as a natural difference in the optical responses of chiral materials with opposite handedness. It stems from the quantised spin angular momentum ±ħ per photon, with the ± representing either left- or right-handed circular polarisations. Less well known, until recently, was the possibility that matter might also respond in a similar, discriminatory way to the handedness of twisted light, or ‘optical vortices’, whose orbital angular momentum (OAM) is quantised as ℓ ℏ per photon, where ℓ is the topological charge whose sign determines a wavefront twist to the left or right. Initial studies focusing on whether, in spectroscopic applications, chiral matter might respond differently to the vortex handedness of + ℓ and − ℓ beams, failed to identify any viable mechanism. However, in the last few years, theory and experiment have both supplied ample evidence that, under certain conditions, such forms of interaction do exist—and as a result, the field of chirality and optical OAM is beginning to flourish at a pace. This topical review presents a survey of this new field, working up from a description of those initial studies to the cutting-edge experiments now taking place. Analysing the fundamental mechanisms provides for a revision of previous precepts, broadening their scope in the light of recent advances in understanding, and highlighting a vibrant synergy between the fields of optical activity and twisted light.

Raman optical activity underpins a powerful vibrational spectroscopic technique for obtaining detailed structural information about chiral molecular species. The effect centers on the discriminatory interplay between the handedness of material chirality with that of circularly polarized light. Twisted light possessing an optical orbital angular momentum carries helical phase fronts that screw either clockwise or anticlockwise and, thus, possess a handedness that is completely distinct from the polarization. Here a novel form of Raman optical activity that is sensitive to the handedness of the incident twisted photons through a spin-orbit interaction of light is identified, representing a new chiroptical spectroscopic technique.

Optical binding is a laser‐induced inter‐particle force that exists between two or more particles subjected to off‐resonant light. It is one of the key tools in optical manipulation of particles. Distinct from the single‐particle forces which operate in optical trapping and tweezing, it enables the light‐induced self‐assembly of non‐contact multi‐particle arrays and structures. Whilst optical binding at the microscale between microparticles is well‐established, it is only within the last few years that the experimental difficulties of observing nanoscale optical binding between nanoparticles have been overcome. This hurdle surmounted, there has been a sudden proliferation in observations of nanoscale optical binding, where the corresponding theoretical understanding and predictions of the underlying nanophotonics have become ever more important. This article covers these new developments, giving an overview of the emergent field of nanoscale optical binding.

Circular dichroism is the differential rate of absorption of right- and left-handed circularly polarized light by chiral particles. Optical vortices which convey orbital angular momentum (OAM) possess a chirality associated with the clockwise or anticlockwise twisting of their wave front. Here it is highlighted that both oriented and randomly oriented chiral particles absorb photons from twisted beams at different rates depending on whether the vortex twists to the right or the left through a dipole coupling scheme. This is in contrast to previous studies that investigated dipole couplings with vortex modes in the paraxial approximation and showed no such chiral sensitivity to the vortex handedness: only in oriented media where electric quadrupole coupling contributes to optical activity effects due to absorption does such a mechanism exist for paraxial vortices. The distinct difference in the scheme highlighted in this work is that longitudinal fields are taken into account. Due to the vortex dichroism persisting in randomly oriented collections of chiral particles, the mechanism has a distinct advantage in its potential applicability in chemical and biochemical applications where the systems under study are invariably in the liquid phase. Additionally, the result is put into context in terms of the quantifiable optical chirality, highlighting that optical OAM can in fact increase the optical chirality density of an electromagnetic field.

Recent molecular photonics studies have highlighted the significant role that phase-structured light possessing orbital angular momentum (OAM) can have when interacting with matter. These studies discovered chiroptical effects sensitive to both the magnitude and sign of the optical OAM in both the absorption and scattering of twisted photons by molecules and nanoparticles. Specifically, it has been shown how a structured beam engaging with electric-quadrupole transitions in the material allows a unique sensitivity to the helical-phase structure of twisted light. In this paper we highlight experimental methodologies and systems suitable to observe and quantify the chiroptical processes of Rayleigh and Raman optical activity, and the newly discovered circular-vortex differential scattering effect with structured light—including the importance of off-axis beam alignment, input beam intensity structure, multipolar moments, and scattering-angle dependencies. It is shown that with a judicious choice of experimental setup, chiroptical effects that scale with the topological charge $\ell$ or OAM of the input beam enable optical activity signals to be enhanced and significantly exceed those based solely on circularly polarized, unstructured light. The new technique thus offers a highly useful and important spectroscopic application of structured light. The more detailed role that perfect optical vortices with high OAM will play in such optical activity effects is now highlighted, to show where there is substantial scope for experimental application, specifically in vibrational optical activity and chiral spectroscopy.