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 present the new planar extrinsic chirality metamaterial (ECM) design that manifests giant circular dichroism (CD) in the visible spectrum range rather than usual near-infrared and terahertz range. Effects of incident beam angles and meta-molecules unit sizes on the CD spectrums were theoretically analyzed; Physical mechanism was illustrated in new figures of asymmetrical current excitation in neighboring unit cells.
We investigate a geometrically symmetric gold-silicon sphere heterodimer and reveal its extrinsic chiroptical response caused by the interaction with a substrate. The chiroptical response is obtained for oblique incidence owing to the coalescence of extrinsic chirality, heterogeneity and substrate induced break of symmetry. To quantify the chiral response we utilize k-space polarimetry. We elucidate the physics of the involved phenomena by considering scattering properties of the heterodimer in free space and find that incident linearly polarized light is scattered in a spin-split fashion. We …
We propose a framework that connects the spatial symmetries of a metasurface to its material parameter tensors and its scattering matrix. This provides a simple yet effective way to effortlessly determine properties of a metasurface scattering response, such as chirality or asymmetric transmission, and which of its effective material parameters should be taken into account in the prospect of a homogenization procedure. In contrast to existing techniques, this approach does not require any a priori knowledge of group theory or complicated numerical simulation schemes, hence making it fast, easy…
We present the characteristics of a simple waveguiding structure constructed by anisotropic birefringent crystal-metal-chiral medium, anisotropic-metal-chiral in short, and reveal the chiral-dependent dispersion and propagation properties of the surface plasmon polaritons (SPPs). We demonstrate its remarkable discrimination ability to the magnitude and sign of both the real and imaginary part of the chirality parameter. The anisotropy plays a key role in such performance and shows tuneable ability in enantiomeric discrimination even when the chirality parameter is complex-valued. Most importan…
Spin-multiplexed terahertz image edge detection based on extrinsic chirality in all-dielectric metasurface
Sichuan Province Key Laboratory of Optoelectronic Sensor Devices and Systems, College of Optoelectronic Engineering (Chengdu IC Valley Industrial College), Chengdu University of Information Technology(成都信息工程大学光电工程学院(成都IC谷产业学院));Sichuan Meteorological Optoelectronic Sensor Technology and Application Engineering Research Center, Chengdu University of Information Technology(成都信息工程大学四川省气象光电传感器技术与应用工程研究中心);School of Precision Instruments and Opto-Electronics Engineering, Tianjin University(天津大学精密仪器与光电子工程学院)
We suggest that all-photodesigned metamaterials, sub-wavelength custom patterns of photo-excited carriers on a semiconductor, can display an exotic extrinsic electromagnetic chirality in terahertz (THz) frequency range. We consider a photo-induced pattern exhibiting 1D geometrical chirality, i.e. its mirror image can not be superposed onto itself by translations without rotations and, in the long wavelength limit, we evaluate its bianisotropic response. The photo-induced extrinsic chirality turns out to be fully reconfigurable by recasting the optical illumination which supports the photo-exci…
Circular dichroism is widely used for characterizing organic and biological materials, but measurements at a single molecule level are challenging because differences in absorption for opposite helicities are small. Here we show that extrinsic chirality can induce giant circular dichroism in individual carbon nanotubes, with degree of polarization reaching 65%. The signal has a large dependence on the incidence angle, consistent with the interpretation that mirror symmetry breaking by the optical wave vector is responsible for the effect. We propose that field-induced charge distribution resul…
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…
In this work, the circular dichroisms (CD) of nanorice heterodimers consisting of two parallel arranged nanorices with the same size but different materials are investigated theoretically. Symmetry-breaking is introduced by using different materials and oblique incidence to achieve strong CD at the vicinity of Fano resonance peaks. We demonstrate that all Au-Ag heterodimers exhibit multipolar Fano resonances and strong CD effect. A simple quantitative analysis shows that the structure with larger Fano asymmetry factor has stronger CD. The intensity and peak positions of the CD effect can be fl…
Kirigami-based Flexible Metasurface with Reconfigurable Intrinsic Chirality from Zero to Near-unity
The Hong Kong University of Science and Technology (Guangzhou)(香港科技大学(广州));Low Altitude Systems and Economy Research Institute, The Hong Kong University of Science and Technology (Guangzhou)(香港科技大学(广州)低空经济与系统研究院);Wuhan University of Technology(武汉理工大学)
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…
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…
We design, in a most simple way, Fabry-Perot cavities with longitudinal chiral modes by sandwiching between two smooth metallic silver mirrors a layer of polystyrene made planar chiral by torsional shear stress. We demonstrate that the helicity-preserving features of our cavities stem from a spin-orbit coupling mechanism seeded inside the cavities by the specific chiroptical features of planar chirality. Planar chirality gives rise to an extrinsic source of three-dimensional chirality under oblique illumination that endows the cavities with enantiomorphic signatures measured experimentally and…
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 …
We demonstrate natural optical activity in disordered ensembles of non-chiral plasmonic resonators. We show that the statistical distributions of rotatory power and spatial dichroism are strongly dependent on the scattering mean free path in diffusive random media. This result is explained in terms of the intrinsic geometric chirality of disordered media, as they lack mirror symmetry. We argue that chirality and natural optical activity of disordered systems can be quantified by the standard deviation of both rotatory power and spatial dichroism. Our results are based on microscopic electromag…
Chiral optical effects are generally quantified along some specific incident directions of exciting waves (especially for extrinsic chiralities of achiral structures) or defined as direction-independent properties by averaging the responses among all structure orientations. Though of great significance for various applications, chirality extremization (maximized or minimized) with respect to incident directions or structure orientations have not been explored, especially in a systematic manner. In this study we examine the chiral responses of open photonic structures from perspectives of quasi…
Chirality Inversion and Giant Optical Activity in Scalable Self-Assembled Metamaterials
Max Planck Institute of Colloids and Interfaces (MPIKG)(马克斯·普朗克胶体与界面研究所);Department of Chemistry, University of Cambridge(剑桥大学化学系);Institute of Light and Matter, Claude Bernard University Lyon 1, CNRS(里昂第一大学克劳德·贝尔纳大学光与物质研究所,法国国家科学研究中心)
Recently it was discovered that periodic lattices of metamaterial scatterers show optical activity, even if the scatterers or lattice show no 2D or 3D chirality, if the illumination breaks symmetry. In this Letter we demonstrate that such `pseudo-chirality' is intrinsic to any single planar metamaterial scatterer and in fact has a well-defined value at a universal bound. We argue that in any circuit model, a nonzero electric and magnetic polarizability derived from a single resonance automatically imply strong bianisotropy, i.e., magneto-electric cross polarizability at the universal bound set…
Prospects of using metal hole arrays for the enhanced optical detection of molecular chirality in nanosize volumes are investigated. Light transmission through the holes filled with an optically active material is modeled and the activity enhancement by more than an order of magnitude is demonstrated. The spatial resolution of the chirality detection is shown to be of a few tens of nanometers. From comparing the effect in arrays of cylindrical holes and holes of complex chiral shape, it is concluded that the detection sensitivity is determined by the plasmonic near field enhancement. The intri…
We report that the classical phenomena of optical activity and circular dichroism, which are traditionally associated with chirality (helicity) of organic molecules, proteins and inorganic structures, can be observed in non-chiral artificial media. Intriguingly, our metamaterial structure yields exceptionally strong resonant optical activity, which also leads to the appearance of a backward wave, a characteristic sign of negative-index media.
In this article the concept of enantiomorphism is developed in terms of topological, rather than geometrical, concepts. Chirality is to be associated with enantiomorphic pairs which induce Optical Activity, while Helicity is to be associated enantiomorphic pairs which induce a Faraday effect. Experimentally, the existence of enantiomorphic pairs is associated with the lack of a center of symmetry, which is also serves as a necessary condition for Optical Activity. However, Faraday effects may or may not require a lack of a center of symmetry. The two species of enantiomorphic pairs are distinc…
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 …
We report extremely strong optical activity and circular dichroism exhibited by subwavelength arrays of four-start-screw holes fabricated with one-pass focused ion beam milling of freely suspended silver films. Having the fourth order rotational symmetry, the structures exhibit the polarization rotation up to 90 degrees and peaks of full circular dichroism and operate as circular polarizers within certain ranges of wavelengths in the visible. We discuss the observations on the basis of general principles (symmetry, reciprocity and reversibility) and conclude that the extreme optical chirality …
Conventional linear optical activity effects are widely used for studying chiral materials. However, poor contrast and artifacts due to sample anisotropy limit the applicability of these methods. Here we demonstrate that nonlinear second-harmonic-generation circular dichroism spectral microscopy can overcome these limits. In intact collagenous tissues, clear spectral resonance is observed with sub-micrometer spatial resolution. By performing gradual protein denaturation studies, we show that the resonant responses are dominantly due to the molecular chirality.
Using terahertz time domain spectroscopy we demonstrate tunable polarization rotation and circular dichroism in intrinsically nonchiral planar terahertz metamaterials without twofold rotational symmetry. The observed effect is due to extrinsic chirality arising from the mutual orientation of the metamaterial plane and the propagation direction of the incident terahertz wave.
A bilayered chiral metamaterial (CMM) is proposed to realize a 90 degree polarization rotator, whose giant optical activity is due to the transverse magnetic dipole coupling among the metallic wire pairs of enantiomeric patterns. By transmission through this thin bilayered structure of less than λ/30 thick, a linearly polarized wave is converted to its cross polarization with a resonant polarization conversion efficiency (PCE) of over 90%. Meanwhile, the axial ratio of the transmitted wave is better than 40 dB. It is demonstrated that the chirality in the propagation direction makes this effic…
We demonstrated a 2D helical chiral metamaterial that exhibits broadband strong optical activity resulting nonresonant Drude-like response. The strong chirality leads to broadband negative refractive index with high figure of merit (>90) and extremely low loss (<2% per layer). The optical activity are insensitive to the angles of incident electromagnetic waves, thereby enabling more flexibility in polarization manipulation applicaitons.
The optical properties of nanoparticle clusters vary with the spatial arrangement of the constituent particles, but also the overall orientation of the cluster with respect to the incident light. This is particularly important in the context of nanoscale chirality and associated chiroptical responses, such as circular dichroism or differential scattering of circularly polarised light in the far-field, or local degree of optical chirality in the near-field. We explore the angular dependence of such quantities for a few archetypal geometries: a dimer of gold nanorods, a helix of gold nanospheres…
We demonstrate numerically and experimentally a conjugated gammadion chiral metamaterial that uniaxially exhibits huge optical activity and circular dichroism, and gives a negative refractive index. This chiral design provides smaller unit cell size and larger chirality compared with other published planar designs. Experiments are performed at GHz frequencies (around 6GHz) and in good agreement with the numerical simulations.
The combination of gain and loss in optical systems that respect parity-time (PT)-symmetry has pointed recently to a variety of novel optical phenomena and possibilities. Many of them can be realized by combining the PT-symmetry concepts with metamaterials. Here we investigate the case of chiral metamaterials, showing that combination of chiral metamaterials with PT-symmetric gain-loss enables a very rich variety of phenomena and functionalities. Examining a simple one-dimensional chiral PT-symmetric system, we show that with normally incident waves the PT-symmetric and the chirality-related c…
Quantifying the optical chirality of a sample requires the precise measurement of the rotation of the plane of linear polarisation of the transmitted light. Central to this notion is that the sample needs to be exposed to light of a defined polarisation state. We show that by using a polarisation-entangled photon source we can measure optical activity whilst illuminating a sample with unpolarised light. This not only allows for low light measurement of optical activity but also allows for the analysis of samples that would otherwise be perturbed if subject to polarised light.
Mirror symmetry is among the most fundamental concepts of physics and its spontaneous breaking at the molecular level allows chiral molecules to exist in two enantiomers that are mirror images of each other. The majority of chiro-optical effects routinely used to detect enantiomers in mixtures, as circular dichroism, relies on chiral sensitivity to photon circular polarization, thus not harnessing the full potentials of mirror symmetry breaking which also involves the radiation spatial profile. Here we show that the parity indefiniteness of the electromagnetic field interacting with chiral mat…
Motivated by the theoretical observation that isotropic chirality can exist even in completely random systems, we design a dielectric metamaterial consisting of a random colloid of meta-atoms, which exhibits unprecedentedly high isotropic optical activity. Each meta-atom is composed of a helically arranged cluster of silicon nanospheres. Such clusters can be fabricated by large-scale DNA self-assembly techniques. It is demonstrated that the use of a high concentration of the meta-atoms in the colloid provides significant suppressions of incoherent scattering losses. As a result, the proposed s…
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 anti-clockwise twisting of their wavefront. 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 wit…
Complex systems with coexisting polarity, chirality and incommensurate magnetism are of great interest because they open new degrees of freedom in interaction between different subsystems and therefore they host a plethora of intriguing physical properties. Here we report on optical properties and lattice and spin dynamics of Ni$_2$InSbO$_6$ single crystals studied with the use of polarized optical microscopy and micro-Raman spectroscopy in the temperature range 10-300 K. Ni$_2$InSbO$_6$ crystallizes in a polar structure described by the noncentrosymmetric space group R3 and two types of struc…