It has been long recognized that the spatial polarization of the electronic clouds in molecules, and the spatial arrangements of atoms into chiral molecular structures, play crucial roles in physics, chemistry and biology. However, these two fundamental concepts - chirality and polarization - have remained unrelated so far. This work connects them by introducing and exploring the concept of polarization of chirality. We show that, like charge, chirality, or handedness, can be polarized, and that such polarization leads to fundamental consequences, demonstrated here using light. First, we analyze how chirality dipoles and higher-order chirality multipoles manifest in experimental observables. Next, we show how to create chirality-polarized optical fields of alternating handedness in space. Despite being achiral, these racemic space-time light structures interact differently with chiral matter of opposite handedness, and the chirality dipole of light controls and quantifies the strength of the enantio-sensitive response. Using nonlinear interactions, we can make a medium of randomly oriented chiral molecules emit light to the left, or to the right, depending on the molecular handedness and on the chirality dipole of light. The chiral dichroism in emission direction reaches its highest possible value of 200%. Our work opens the field of chirality polarization shaping of light and new opportunities for efficient chiral discrimination and control of chiral and chirality-polarized light and matter on ultrafast time scales.
Synthetic chiral light enables ultrafast and highly efficient imaging of molecular chirality. Unlike standard circularly polarized light, the handedness of synthetic chiral light does not rely on the spatial structure of the light field: it is encoded locally, in the chiral trajectory that the tip of the electric-field vector draws in time, at each point in space. Being locally chiral, already within the electric-dipole approximation, synthetic chiral light is a highly efficient chiral photonic reagent. Synthetic chiral light that is locally and globally chiral allows us to selectively quench …
Synthetic chiral light fields were recently introduced as a novel source of chirality [Ayuso et al. Nat. Phot. 13, 866 (2019)]. This locally-chiral light spans a three-dimensional polarization that plots a chiral trajectory in space-time, leading to huge nonlinear chiral signals upon interactions with chiral media. The degree of chirality of this new form of light was defined, characterized, and shown to be proportional to the chiral signal conversion efficiency. However, the sign of the light's chirality - its 'handedness' - has not yet been defined. Standard definitions of helicity are inapp…
Geometrical chirality is a universal property encountered on very different length scales ranging from geometrical shapes of living organisms to protein and DNA molecules. Interaction of chiral matter with chiral light - that is, electromagnetic field possessing a certain handedness - underlies our ability to discriminate enantiomers of chiral molecules. In this context, it is often desired to have an optical cavity that efficiently couples to only a specific (right or left) molecular enantiomer, and does not couple to the opposite one. Here, we demonstrate a single-handedness chiral optical c…
The occurrence of biological homochirality is attributed to symmetry breaking mechanisms which are still debatable1. Studies of symmetry breaking require tools for monitoring the population ratios of individual chiral nano-objects, such as molecules, polymers or nanocrystals. Moreover, mapping their spatial distributions may elucidate on the symmetry breaking mechanism. Recently, researchers have utilized differential scattering or circular dichroism microscopy to identify chirality on individual plasmonic nanostructures and inorganic nanocrystals. However, these measurements are prone to opti…
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…
We investigate the plasmonic nanohelix as an individual subwavelength element for locally probing light chirality. We show that an hybrid nanoantenna combining a carbon-gold core-shell helix and a plasmonic nanoaperture transmits circularly polarized light with the same handedness as the helix and blocks the other. Such an assymmetric response is spatially localized, spectrally broadband and background-free. Finally, we demonstrate the possibility to engineer an individual plasmonic helix at the apex of a sharp tip typically used in scanning near-field microscopies, thus opening the prospect o…
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…
Structural chirality can induce counter-intuitive optical forces due to inherent symmetry properties. While optical forces on a single chiral particle in the Rayleigh regime have been well studied, optical forces in coupled chiral particles remain less explored. By using full-wave numerical simulations and analytical methods of source representation and coupled mode theory, we investigated the optical forces induced by a plane wave on two chiral particles coupling with each other via the evanescent near fields. We found that the induced electric and magnetic dipoles of the chiral particles hav…
Atoms are usually thought of as achiral objects. However, one can construct superpositions of atomic states that are chiral [1]. Here we show how to excite such superpositions with tailored light fields both in the weak-field and strong-field regimes, using realistic laser parameters. First, we use time-dependent Schrodinger equation (TDSE) simulations to demonstrate the creation of a time-dependent bound chiral wavepacket in sodium atoms. Second, we show how the time-dependent handedness of this wavepacket can be probed by photoelectron circular dichroism, in spite of the central symmetry of …
Many nanophotonic applications require precise control and characterization of electromagnetic field properties at the nanoscale. The chiral properties of the field are among its key characteristics, yet measurement of optical chirality at dimensions beyond the diffraction limit has proven difficult. Here we theoretically show that the chiral properties of light can be characterized down to the nanometer scale by means of force detection. To measure the chiral properties of a beam of given handedness at the nanoscale, we determine the photo-induced force exerted on a sharp tip, which is illumi…
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…
We introduce and theoretically analyze the concept of manipulating optical chirality via strong coupling of the optical modes of chiral nanostructures with excitonic transitions in molecular layers or semiconductors. With chirality being omnipresent in chemistry and biomedicine, and highly desirable for technological applications related to efficient light manipulation, the design of nanophotonic architectures that sense the handedness of molecules or generate the desired light polarization in an externally controllable manner is of major interdisciplinary importance. Here we propose that such…
The axial propagation of circularly polarized light in an optically active structurally chiral medium is exactly solved via full electromagnetic analysis. Some symmetries of the system's characteristic matrix reveal new insights, which are confirmed by coupled wave theory. For extreme values of chirality, now accessible via metamaterials, a reverse circular Bragg resonance arises in the negative refraction regime where handedness reversal of counterpart modes occurs. A condition is identified under which optical activity offsets structural chirality, rendering the medium simply birefringent.
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）
We introduce a microscopy technique that facilitates the prediction of spatial features of chirality of nanoscale samples by exploiting photo-induced optical force exerted on an achiral tip in the vicinity of the test specimen. The tip-sample interactive system is illuminated by structured light to probe both the transverse and longitudinal (with respect to the beam propagation direction) components of the sample magnetoelectric polarizability as the manifestation of its sense of handedness, i.e., chirality. We specifically prove that although circularly polarized waves are adequate to detect …
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…
Tunable high-$Q$ Janus-to-chiral bound states in the continuum in bilayer PhCs
School of Physics and Optoelectronics, Xiangtan University（湘潭大学物理与光电工程学院）；School of Physics and Electronics, Hunan University（湖南大学物理学院）；State Key Laboratory of Millimeter Waves, Southeast University（东南大学毫米波国家重点实验室）；Science, Mathematics and Technology (SMT) Cluster, Singapore University of Technology and Design（新加坡科技设计大学科学、数学与技术学部）
We put forward an enantioselective method for chiral nanoparticles using optical tweezers. We demonstrate that the optical trapping force in a typical, realistic optical tweezing setup with circularly-polarized trapping beams is sensitive to the chirality of core-shell nanoparticles, allowing for efficient enantioselection. It turns out that the handedness of the trapped particles can be selected by choosing the appropriate circular polarization of the trapping beam. The chirality of each individual trapped nanoparticle can be characterized by measuring the rotation of the equilibrium position…
Photons experience mirror asymmetry of macroscopic chiral media, as in circular dichroism and polarization rotation, since left and right handed circular polarizations differently couple with matter handedness. Conversely, free relativistic electrons with vanishing orbital angular momentum have no handedness so the question arises whether they could sense chirality of geometrically symmetric macroscopic samples. In this Letter, we show that matter chirality breaks mirror symmetry of the scattered electrons quantum decoherence, even when the incident electron wave function and the sample shape …
Optical systems with gain and loss that respect Parity-Time (PT) symmetry can have real eigenvalues despite their non-Hermitian character. Chiral systems impose circularly polarized waves which do not preserve their handedness under the combined space- and time- reversal operations and, as a result, seem to be incompatible with systems possessing PT symmetry. Nevertheless, in this work we show that in certain configurations, PT symmetric permittivity, permeability and chirality is possible; in addition, real eigenvalues are maintained even if the chirality goes well beyond PT symmetry. By obta…
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 report observation of electron helical dichroism on a material with chiral structure. In analogy with circular dichroism, a common technique for molecular structural fingerprinting, we use a nanofabricated forked diffraction grating to prepare electron vortex beams with opposite orbital angular momenta incident upon metal nanoparticle clusters and post-select for a zero-orbital angular momentum final state. We observe a difference in the differential scattering probability for orbital angular momentum transfer from vortices with opposite handedness incident on chiral aluminum nanoparticle c…
Propagation of light through a thin flat metallic screen containing a hole of twisted shape is sensitive to whether the incident wave is left or right circularly polarized. The transmitted light accrues a component with handedness opposite to the incident wave. The efficiency of polarization conversion depends on the mutual direction of the hole's twist and the incident light's wave polarization handedness and peaks at a wavelength close to the hole overall size. We also observed a strong transmitted field concentration at the center of the chiral hole when the handedness of the chiral hole an…
Planar chiral nanoantenna for excitation-chirality-controlled hot spot modulation and emitter-coupled circularly polarized emission
Friedrich Schiller University Jena（耶拿弗里德里希·席勒大学）；Abbe Center of Photonics, Friedrich Schiller University Jena（耶拿弗里德里希·席勒大学阿贝光学中心）；Leibniz Institute of Photonic Technology（莱布尼茨光子技术研究所）；University of Würzburg（维尔茨堡大学）；The Australian National University（澳大利亚国立大学）；Academia Sinica（中央研究院）；National Yang Ming Chiao Tung University（国立阳明交通大学）
Using the phenomena of linear and circular birefringence we propose a device that can alter general elliptical polarization of a beam by a predetermined amount, thereby allowing conversion between linearly-polarized light and circularly polarized light or changes to the handedness of the polarization. Based on an analogy with two-state adiabatic following of quantum optics, the proposed device is insensitive to the frequency of the light -- it serves as an achromatic polarization retarder.
Characterizing chirality is highly important for applications in the pharmaceutical industry, as well as in the study of dynamical chemical and biological systems. However, this task has remained challenging, especially due to the ongoing increasing complexity and size of the molecular structure of drugs and active compounds. In particular, large molecules with many active chirality centers are today ubiquitous, but remain difficult to structurally analyze due to their high number of stereoisomers. Here we theoretically explore the sensitivity of high harmonic generation (HHG) to the chirality…
Chiral surface plasmon polaritons (SPPs) can be generated by linearly polarized light incident at the end of a nanowire, exciting a coherent superposition of three specific nanowire waveguide modes. Images of chiral SPPs on individual nanowires obtained from quantum dot fluorescence excited by the SPP evanescent field reveal the chirality predicted in our theoretical model. The handedness and spatial extent of the helical periods of the chiral SPPs depend on the input polarization angle and nanowire diameter as well as the dielectric environment. Chirality is preserved in the free-space output…
Photons are nonchiral particles: their handedness can be both left and right. However, when light is transversely confined, it can locally exhibit a transverse spin whose orientation is fixed by the propagation direction of the photons. Confined photons thus have chiral character. Here, we employ this to demonstrate nonreciprocal transmission of light at the single-photon level through a silica nanofibre in two experimental schemes. We either use an ensemble of spin-polarised atoms that is weakly coupled to the nanofibre-guided mode or a single spin-polarised atom strongly coupled to the nanof…
