We examine the recently introduced measure of chirality of a monochromatic optical field [Y. Tang and A. E. Cohen, Phys. Rev. Lett. 104, 163901 (2010)] using the momentum (plane-wave) representation and helicity basis. Our analysis clarifies the physical meaning of the measure of chirality and unveils its close relation to the polarization helicity, spin angular momentum, energy density, and Poynting energy flow. We derive the operators of the optical chirality and of the corresponding chiral momentum, which acquire remarkably simple forms in the helicity representation.
Geometrical chirality is a property of objects that describes three-dimensional mirror-symmetry violation and therefore it requires a non-vanishing spatial extent. In contrary, optical chirality describes only the local handedness of electromagnetic fields and neglects the spatial geometrical structure of optical beams. In this manuscript, we put forward the physical significance of geometrical chirality of spatial structure of optical beams, which we term "Kelvin's chirality". Further, we report on an experiment revealing the coupling of Kelvin's chirality to optical chirality upon transmissi…
It has been assumed that optical activity can be measured by illuminating alternatively a material with left- and right- handed circular polarized light and analyzing the differential response. This simple and intuitive approach is in general incorrect, and has led to misleading idea that extrinsic chirality involves optical activity.
We derived an analytical formula for the optical force acting on a small anisotropic chiral particle. The behavior of chiral particles is qualitatively different from achiral particles due to new chirality dependent terms which couple mechanical linear momentum and optical spin angular momentum. Such coupling induced by chirality can serve as a new mechanism to achieve optical pulling force. Our analytical predictions are verified by numerical simulations.
We report on a numerical study of optical chirality. Intertwined gold helices illuminated with plane waves concentrate right and left circularly polarized electromagnetic field energy to sub-wavelength regions. These spots of enhanced chirality can be smoothly shifted in position and magnitude by varying illumination parameters, allowing for the control of light-matter interactions on a nanometer scale.
Recently, Tang and Cohen (Science 332, 333, 2011) have demonstrated a scheme to enhance the chiral response of molecules, which relies on the use of circularly polarized light in a standing wave configuration. Here we show a new type of light which possesses orbital angular momentum and enhanced chiral response. Unexpectedly, in the locations where the beams show enhanced optical chirality, only the longitudinal components of the electric and magnetic fields survive, showing a new way to yield optical chirality different from the usual.
Several dynamical properties such as energy, momentum, angular momentum, and optical helicity have been recently reexamined in dispersive and lossless media. Here, we address a parallel derivation for the optical chirality, extending it so as to include dissipative effects as well. To this end, we first elaborate on the most complete form of the conservation law for the optical chirality, without any restrictions on the nature of the medium. As a result we find a general expression for the optical chirality density both in lossless and lossy dispersive media. Our definition is perfectly consis…
Analytical forms of the optical helicity and optical chirality of monochromatic Laguerre-Gaussian optical vortex beams are derived up to second order in the paraxial parameter $kw_0$. We show that input linearly polarised optical vortices which possess no optical chirality, helicity or spin densities can acquire them at the focal plane for values of a beam waist $w_0 \approx λ$ via an OAM-SAM conversion which is manifest through longitudinal (with respect to the direction of propagation) fields. We place the results into context with respect to the intrinsic and extrinsic nature of SAM and OAM…
The transverse component of the spin angular momentum of evanescent waves gives rise to lateral optical forces on chiral particles, which have the unusual property of acting in a direction in which there is neither a field gradient nor wave propagation. As their direction and strength depends on the chiral polarizability of the particle, they act as chirality-sorting and may offer a mechanism for passive chirality spectroscopy. The absolute strength of the forces also substantially exceeds that of other recently predicted sideways optical forces, such that they may more readily offer an experi…
Light interacts differently with left and right handed three dimensional chiral objects, like helices, and this leads to the phenomenon known as optical activity. Here, by applying a polarization tomography, we show experimentally, for the first time in the visible domain, that chirality has a different optical manifestation for twisted planar nanostructured metallic objects acting as isolated chiral metaobjects. Our analysis demonstrate how surface plasmons, which are lossy bidimensional electromagnetic waves propagating on top of the structure, can delocalize light information in the just pr…
A whispering gallery mode resonator with a cavity-made slot filled atomic vapor is demonstrated, in which the chiral symmetry is broken induced by asymmetric backscattering of counter-propagating optical waves in the WGM microcavity. The chirality of resonator modes is steered via tuning dispersion relation in the cavity-made slot. The system exhibiting a high displacement sensitivity 15.22 THz/nm could be applied to optomechanical sensing applications.
To optimize the interaction between chiral matter and highly twisted light, quantities that can help characterize chiral electromagnetic fields near nanostructures are needed. Here, by analogy with Poynting's theorem, we formulate the time-averaged conservation law of optical chirality in lossy dispersive media and identify the optical chirality flux as an ideal far-field observable for characterizing chiral optical near fields. Bounded by the conservation law, we show that it provides precise information, unavailable from circular dichroism spectroscopy, on the magnitude and handedness of hig…
The effects of Fano resonance on the optical chirality of planar plasmonic nanodevices in the visible wavelength range are experimentally observed and theoretically explained. The nanodevice consists of a nanodisk at the center with six gold nanorods with an orientation angle to exhibit optical chirality under dark-field illumination. The chiral response induced by the gold nanorods are affected by the presence of the nanodisk with different diameters which causes Fano resonance. An intriguing change to the opposite selection preference of different handedness of the circularly polarized light…
When circularly polarized light interacts with a nanostructure, the optical response depends on the geometry of the structure. If the nanostructure is chiral (i.e., it cannot be superimposed on its mirror image), then its optical response, both in near-field and far-field, depends on the handedness of the incident light. In contrast, achiral structures exhibit identical far-field responses for left- and right-circular polarization. Here, we show that a perfectly achiral nanostructure, a plasmonic metamolecule with trigonal D3h symmetry, exhibits a near-field response that is sensitive to the h…
Chiral nanophotonic devices are promising candidates for chiral molecules sensing, polarization diverse nanophotonics and display technologies. Active chiral nanophotonic devices, where the optical chirality can be controlled by an external stimulus has triggered great research interest. However, efficient modulation of the optical chirality has been challenging. Here, we demonstrate switching of the extrinsic chirality by applied magnetic fields in a magneto-plasmonic metasurface device based on a magneto-optical oxide material, Ce1Y2Fe5O12 (Ce:YIG). Thanks to the low optical loss and strong …
Optical chirality has been recently suggested to complement the physically relevant conserved quantities of the well-known Maxwell's equations. This time-even pseudoscalar is expected to provide further insight in polarization phenomena of electrodynamics such as spectroscopy of chiral molecules. Previously, the corresponding continuity equation was stated for homogeneous lossless media only. We extend the underlying theory to arbitrary setups and analyse piecewise-constant material distributions in particular. Our implementation in a Finite Element Method framework is applied to illustrative …
Chirality is a universal feature in nature, as observed in fermion interactions and DNA helicity. Much attention has been given to chiral interactions of light, not only regarding its physical interpretation but also focusing on intriguing phenomena in excitation, absorption, refraction, and topological phase. Although recent progress in metamaterials has spurred artificial engineering of chirality, most approaches are founded on the same principle of the mixing of electric and magnetic responses. Here we propose nonmagnetic chiral interactions of light based on low-dimensional eigensystems. E…
We study the chirality of periodically poled MgO-doped lithium niobate (MgO:PPLN) by electro-optic (EO) effect. It shows that optical propagation is reciprocal in MgO:PPLN when quasi-phase-matching (QPM) condition is satisfied, which is similar to natural optical active material like quartz. The specific rotation of MgO:PPLN by EO effect is shown to be proportional to the transverse electric field, making large polarization rotation in optical active material with small size possible. We also demonstrate that the chirality of MgO:PPLN can be controlled by external electric field.
Optical chirality (OC) - one of the fundamental quantities of electromagnetic fields - corresponds to the instantaneous chirality of light. It has been utilized for exploring chiral light-matter interactions in linear optics, but has not yet been applied to nonlinear processes. Motivated to explore the role of OC in the generation of helically polarized high-order harmonics and attosecond pulses, we first separate the OC of transversal and paraxial beams to polarization and orbital terms. We find that the polarization-associated OC of attosecond pulses corresponds to that of the pump in the qu…
We demonstrate that nanostructures carefully designed on both sides of a thin suspended metallic membrane couple light into a chiral near field and transmit vortex beams through a central aperture that connects the two sides of the membrane. We show how far-field orbital angular momentum (OAM) indices can be tailored through nanostructure designs. We reveal the crucial importance of OAM selection rules imposed by the central aperture and derive OAM summation rules in perfect agreement with experimental data.
Chirality is a ubiquitous phenomenon in the natural world. Many biomolecules without inversion symmetry such as amino acids and sugars are chiral molecules. Measuring and controlling molecular chirality at a high precision down to the atomic scale are highly desired in physics, chemistry, biology, and medicine, however, have remained challenging. Herein, we achieve all-optical reconfigurable chiral meta-molecules experimentally using metallic and dielectric colloidal particles as artificial atoms or building blocks to serve at least two purposes. One is that the on-demand meta-molecules with s…
We suggest that electromagnetic chirality, generally displayed by 3D or 2D complex chiral structures, can occur in 1D patterned composites whose components are achiral. This feature is highly unexpected in a 1D system which is geometrically achiral since its mirror image can always be superposed onto it by a 180 deg rotation. We analytically evaluate from first principles the bi-anisotropic response of multilayered metamaterials and we show that the chiral tensor is not vanishing if the system is geometrically one-dimensional chiral, i.e. its mirror image can not be superposed onto it by using…
In this text we describe the role of optical chirality in the context of plasmonics. We clearly distinguish between 2D an 3D optical chirality and connect the problem with reciprocity and time symmetry. We compare our analysis with recent experimental results in nano-plasmonics and photonics.
Artificial nanostructures enable fine control of electromagnetic fields at the nanoscale, a possibility that has recently been extended to the interaction between polarised light and chiral matter. The theoretical description of such interactions, and its application to the design of optimised structures for chiroptical spectroscopies, brings new challenges to the common set of tools used in nano-optics. In particular, chiroptical effects often depend crucially on the relative orientation of the scatterer and the incident light, but many experiments are performed with randomly-oriented scatter…
The local chiral symmetry between clockwise (CW) and counter-clockwise (CCW) propagating light in a deformed microcavity can be broken by wave optics effects, which become significant as the cavity size approaches the wavelength. We show that the spatial separation of the CW and CCW ray orbits underlying the high quality factor resonant modes results in unidirectional emission in free space. In the presence of a waveguide, evanescent coupling also becomes directional, and the output direction can be varied by selecting the coupling position along the cavity boundary. Our results demonstrate th…
We present a new design of plasmonic nanoantenna with a slant gap for optical chirality engineering. At resonance, the slant gap provides highly enhanced electric field parallel to external magnetic field with a phase delay of 90 degree, resulting in enhanced optical chirality. We show by numerical simulations that upon linearly polarized excitation our achiral nanoantenna can generate near field with enhanced optical chirality that can be tuned by the slant angle and resonance condition. Our design can be easily realized and may find applications in circular dichroism enhancement.
We analyze how chirality can generate pulling optical forces and left-handed torques by cross-coupling linear-to-angular momenta between the light field and the chiral object. In the dipolar regime, we reveal that such effects can emerge from a competition between non-chiral and chiral contributions to dissipative optical forces and torques, a competition balanced by the strength of chirality of the object. We extend the analysis to large chiral spheres where the interplay between chirality and multipolar resonances can give rise to a break of symmetry that flips the signs of both optical forc…
Dark-field illumination is shown to make planar chiral nanoparticle arrangements exhibit circular dichroism in extinction analogous to true chiral scatterers. Circular dichrosim is experimentally observed at the maximum scattering of single oligomers consisting rotationally symmetric arrangements of gold nanorods, with strong agreement to numerical simulation. A dipole model is developed to show that this effect is caused by a difference in the geometric projection of a nanorod onto the handed orientation of electric fields created by a circularly polarized dark-field that is normally incident…
Optical Control of Chirality by Ultrafast Symmetry Breaking in Membrane Metasurfaces
École Polytechnique Fédérale de Lausanne (EPFL)（洛桑联邦理工学院）；Shubnikov Institute of Crystallography, NRC “Kurchatov Institute”（库尔恰托夫国家研究中心舒比尼科夫晶体学研究所）；School of Physics and Engineering, ITMO University（ITMO大学物理与工程学院）；University of Brescia（布雷西亚大学）；Qingdao Innovation and Development Center, Harbin Engineering University（哈尔滨工程大学青岛创新发展基地）；Theoretical Physics and Quantum Technologies Department, National University of Science and Technology ‘MISIS’（莫斯科国立科学技术大学“MISIS”理论与量子技术系）
We demonstrate that the fundamental causality principle being applied to strongly chiral artificial materials yields the generalized Kramers-Kronig relations for the observables -- circular dichroism and optical activity. The relations include the Blaschke terms determined by material-specific features - the zeros of transmission amplitude on the complex frequency plane. By the example of subwavelength arrays of chiral holes in silver films we show that the causality relations can be used not only for a precise verification of experimental data but also for resolving the positions of material …
Chirality is ubiquitous from microscopic to macroscopic phenomena in physics and biology, such as fermionic interactions and DNA duplication. In photonics, chirality has traditionally represented differentiated optical responses for right and left circular polarizations. This definition of optical chirality in the polarization domain includes handedness-dependent phase velocities or optical absorption inside chiral media, which enable polarimetry for measuring the material concentration and circular dichroism spectroscopy for sensing biological or chemical enantiomers. Recently, the emerging f…
Pseudospin plays a very important role in understanding various interesting physical phenomena associated with 2D materials such as graphene. It has been proposed that pseudospin is directly related to angular momentum, and it was recently experimentally demonstrated that orbit angular momentum is an intrinsic property of pseudospin in a photonic honeycomb lattice. However, in photonics, the interaction between spin and pseudospin for light has never been investigated. In this Letter, we propose that, in an optical analogue of staggered graphene, i.e. a photonic honeycomb lattice waveguide wit…
The possibility to enhance chiral light-matter interactions through plasmonic nanostructures provides entirely new opportunities for greatly improving the detection limits of chiroptical spectroscopies down to the single molecule level. The most pronounced of these chiral interactions occur in the ultraviolet (UV) range of the electromagnetic spectrum, which is difficult to access with conventional localized plasmon resonance based sensors. Although Surface Plasmon Polaritons (SPPs) on noble metal films can sustain resonances in the desired spectral range, their transverse magnetic nature has …
The search for objects that yield maximum electromagnetic chirality in their emitted wavefield has garnered significant attention in recent years. However, achieving such maximum chirality is challenging, as it typically requires complex chiral metamaterials. Here we demonstrate that chiral spheres can yield maximum chirality in their emitted wavefield. Specifically, we analytically find the spectral trajectories at which chiral spheres become optically transparent to a given helicity of the incident field, while for its opposite helicity, they behave as dual objects, i.e., on scattering, they…
We discuss the possibility of enhancing the chiroptical response from molecules uniformly distributed around nanostructures that sustain localized plasmon resonances. We demonstrate that the average optical chirality in the near field of any plasmonic nanostrucure cannot be significantly higher than that in a plane wave. This conclusion stems from the quasi-static nature of the nanoparticle-enhanced electromagnetic fields and from the fact that, at optical frequencies, the magnetic response of matter is much weaker than the electric one.
The realization of lossless metasurfaces with true chirality crucially requires the fabrication of three-dimensional structures, constraining their feasibility for experiments and hampering practical implementations. Even though the three-dimensional assembly of metallic nanostructures has been demonstrated previously, the resulting plasmonic resonances suffer from high intrinsic and radiative losses. The concept of photonic bound states in the continuum (BICs) is instrumental for tailoring radiative losses in diverse geometries, especially when implemented using lossless dielectrics, but appl…
The chirality and helicity of linearly polarised Laguerre-Gaussian (LG) beams are examined. Such a type of light possesses a substantial longitudinal field when its beam waist is sufficiently small and so gives rise to non-zero chirality and helicity. In the simplest case of a doughnut beam of winding number $\ell=1$ and another identical to it but has $\ell= -1$, we obtain different chirality and helicity distributions at the focal plane $z=0$. We also show that this chiral behaviour persists and the patterns evolve so that on planes at $z<0$ and $z>0$ the beam convergence contributes differe…
We derive expressions for the scattering, extinction and conversion of the chirality of monochromatic light scattered by bodies which are characterized by a T-matrix. In analogy to the conditions obtained from the conservation of energy, these quantities enable the classification of arbitrary scattering objects due to their full, i.e. either chiral or achiral, electromagnetic response. To this end, we put forward and determine the concepts of duality and breaking of duality symmetry, anti-duality, helicity variation, helicity annhiliation and the breaking of helicity annihilation. Different cl…
Designing objects with predefined optical properties is a task of fundamental importance for nanophotonics, and chirality is a prototypical example of such a property, with applications ranging from photochemistry to nonlinear photonics. A measure of electromagnetic chirality with a well-defined upper bound has recently been proposed. Here, we optimize the shape of silver helices at discrete frequencies ranging from the far infrared to the optical band. Gaussian process optimization, taking into account also shape derivative information of the helices scattering response, is used to maximize t…
