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Chirality, an intrinsic property of certain entities in the universe, is characterized by the absence of mirror symmetry. Understanding chirality is crucial as it influences molecular interactions and properties. Circular dichroism (CD), measured using circularly polarized light, is a standard technique for probing chirality, but its sensitivity is often limited. Here, we explore extrinsic chirality (i.e. a property arising from asymmetric achiral materials when observed from out of normal incidence directions), using photo-acoustic spectroscopy (PAS). PAS allows direct measurement of local absorption, by monitoring the heat produced and transferred to the surrounding air, regardless the transmitted, reflected, and scattered light that flows away from the sample. In conventional techniques, the CD is usually measured by taking into account only the extinction as transmitted (or reflected) light. In this study, we introduce a new PAS setup that employs an oblique-incidence laser to study extrinsic chirality in silver-coated self-assembled metasurfaces. Our experimental results reveal intriguing CD trends dependent on the angle of incidence and wavelength, indicative of extrinsic chirality. This study expands the application of PAS, enabling simultaneous analysis of multiple wavelengths and providing valuable insights into chiral metasurfaces. [ABSTRACT FROM AUTHOR]

The chiroptical response occurring in the chiral metamaterials (MMs) has crucial and extensive applications for stereochemistry, polarization optics, and spintronics. Yet, such intrinsically chiral metamaterials are restricted to a complicated subwavelength chiral profile, causing pronounced fabrication challenges, particularly at the near‐infrared (N‐IR) spectral regime. Instead, extrinsic chirality can also be observed in the nonchiral MMs under an oblique incidence, indicating that the chiroptical response can be achieved with simple structures. The development of photon‐spin selective integrated devices needs an actively reversible tuning of chirality in MMs. Herein, a reversible switching of the extrinsic chirality at the N‐IR region is demonstrated by integrating a nonvolatile chalcogenide semiconductor, Ge2Sb2Te5, into the nonchiral MMs design. It provides an ultrafast and reconfigurable tuning of transmittance circular dichroism (TCD) between amorphous and crystalline states under a stimulus of a nanosecond pulsed laser at a wavelength of 532 nm. Meanwhile, it also effectively manipulates the TCD by titling both rotation and incident angles while fixing geometrical parameters. Utilizing ellipsometry and analytical inversion, it can obtain not only linear but circular birefringence‐dichroism pairs from a single general ellipsometry measurement, which gives a comprehensive description of the polarization characteristics of the non‐chiral MMs, having an advantage over the typical circular dichroism measurements. [ABSTRACT FROM AUTHOR]

Nanophotonics community has shown great interest in 2D materials because of their unique properties of electromagnetic field manipulation. Many of these materials exhibit strong natural anisotropy, which further opens possibilities of polarization manipulation. Here, we show that α-MoO3, an emerging natural hyperbolic 2D material, can be combined with plasmonic nanostructures to provide strong extrinsic chirality in the visible range. A combination of biaxial anisotropy in α-MoO3 and Fabry–Perot cavities with nanoscale features leads to different absorption of left and right circularly polarized photons, hence exhibiting circular dichroism (CD). Our simulation results predict that multilayer nanoscale-thick films including α-MoO3 are potential candidates for achieving extrinsic chirality across the visible range. Furthermore, we show a significant CD increase when the α-MoO3 layer is coupled with plasmonic nanohole arrays or plasmonic nanocubes. Such designs are achiral in geometry and therefore easier to fabricate. Moreover, we optimize the CD dissymmetry factor gCD for the nanocube-based design at 780 nm, obtaining 84%. We believe that utilizing biaxially anisotropic α-MoO3 films to control and engineer chiro-optical properties in the visible frequency range will open research directions and enable enhanced functionalities in chiro-optical control at the nanoscale, further leading to applications in chiral sensing and CD. [ABSTRACT FROM AUTHOR]

Chiral metamaterials have drawn increasing attention due to their strong chiral responses. Monolayer black phosphorus is a tunable two-dimensional material with anisotropy that plays an important role in a variety of fields such as chirality and polarization control. In this work, we propose a metamaterial with structured monolayer black phosphorus to manipulate the transmission properties of circularly polarized waves. The metamaterial exhibits strong circular dichroism and circular birefringence effects depending on oblique incidence of the circularly polarized wave and has a weaker circular conversion dichroism effect as well. Moreover, this work also investigates effects of different chiral phenomena of the metamaterial on various structural parameters as well as incident angles and the electron concentration. It has been proved that the electron concentration of monolayer black phosphorus can dynamically tune the chirality properties. Remarkably, the non-zero pure optical activity always occurs at one certain frequency regardless of the elevation angle and the azimuthal angle. The proposed framework provides opportunities for designing meta-devices with monolayer black phosphorus and practical potentials for novel and high-performance infrared metamaterials.

Plasmonic chirality, which has garnered significant attention in recent years due to its ability to generate strong near-field enhancement and giant circular dichroism (CD). Currently, various theories have been proposed to explain plasmonic extrinsic chirality, however, a comprehensively quantitative explanation for the high-order optical response of extrinsic metamolecule has yet to be established. Herein, we present a concise and quantitative explanation of the giant high-order extrinsic CD of a plasmonic nanocrescent, which origins from multipole decomposition in combination with the optical theorem. Our findings indicate that the high-order resonance modes exhibit giant CD comparable to dipolar modes and can be conveniently applied to the chiral recognition of metamolecules. Furthermore, the nonradiative electric quadrupole resonance exhibits enormous electric field enhancement near metamolecule, which has great application potential in the fields of molecular recognition and sensing in the visible region.

Abstract Circular dichroism (CD) is an interesting phenomenon originating from the interaction of light with chiral molecules or other nanostructures lacking mirror symmetries in three-dimensional (3D) or two-dimensional (2D) space. While the observable effects of optical chirality are very weak in most of the natural materials, they can be designed and significantly enhanced in synthetic chiral structures, where the spatial symmetry of their component are broken on a nanoscale. Therefore, fabrication of composites capable of cheap, time-saving, and giant CD is desirable for the advanced optical technologies. Here, the giant CD of large-area metal nanocrescent array structures was investigated theoretically and experimentally. The largest value of the CD spectrum measured was larger than 0.5, and the CD spectrum was tuned effectively and extensively while maintaining a large peak intensity, which can be attributed to the selective excitation of the lattice surface modes (LSMs) by circularly polarized light. The analysis of the extrinsic chiral structure shows potential applications in chiral molecule sensing and polarizing imaging.

In this paper, a kind of bi-layer extrinsic chiral metamaterial is proposed to realize asymmetric transmission (AT) of circularly polarized waves in the microwave region. We have studied numerically and experimentally the transmission properties of the proposed structure. The results show that under oblique incident wave the asymmetric transmission effect occurs with a 1.5 GHz operation band. The maximum value of AT parameter reaches up to 0.68 at the resonant frequency, which is larger than those in the extrinsic chiral metamaterials previously reported. This AT phenomenon is illustrated by the surface current distribution in detail. The transmission properties of the incident waves can be dynamically regulated by tuning the incident angles θ and ϕ. This metamaterial is potential in the polarization control applications. [ABSTRACT FROM AUTHOR]

Circular dichroism (CD) is an interesting phenomenon originating from the interaction of light with chiral molecules or other nanostructures lacking mirror symmetries in three-dimensional (3D) or two-dimensional (2D) space. While the observable effects of optical chirality are very weak in most of the natural materials, they can be designed and significantly enhanced in synthetic chiral structures, where the spatial symmetry of their component are broken on a nanoscale. Therefore, fabrication of composites capable of cheap, time-saving, and giant CD is desirable for the advanced optical technologies. Here, the giant CD of large-area metal nanocrescent array structures was investigated theoretically and experimentally. The largest value of the CD spectrum measured was larger than 0.5, and the CD spectrum was tuned effectively and extensively while maintaining a large peak intensity, which can be attributed to the selective excitation of the lattice surface modes (LSMs) by circularly polarized light. The analysis of the extrinsic chiral structure shows potential applications in chiral molecule sensing and polarizing imaging. [ABSTRACT FROM AUTHOR]

The extrinsic chiral metam ate rial has attracted more and more attention as it is a kind of metam ate rial which is simple in structure ？ easy to manufacture ？ and can change the electromagnetic properties by adjusting the angle of incident wave. To this paper, the background and concept of extrinsic chiral metamaterials were briefly introduced ？ and the research progress of the simulation and experiment in microwave ？ terahertz and optical band were focused on, am ing to reveal the practical applications in photonic devices and biomedicine. [ABSTRACT FROM AUTHOR]

Optical circular dichroism (CD) is an important phenomenon in nanophotonics, that addresses top level applications such as circular polarized photon generation in optics, enantiomeric recognition in biophotonics and so on. Chiral nanostructures can lead to high CD, but the fabrication process usually requires a large effort, and extrinsic chiral samples can be produced by simpler techniques. Glancing angle deposition of gold on GaAs nanowires can (NWs) induces a symmetry breaking that leads to an optical CD response that mimics chiral behavior. The GaAs NWs have been fabricated by a self-catalyzed, bottom-up approach, leading to large surfaces and high-quality samples at a relatively low cost. Here, we investigate the second harmonic generation circular dichroism (SHG-CD) signal on GaAs nanowires partially covered with Au. SHG is a nonlinear process of even order, and thus extremely sensitive to symmetry breaking. Therefore, the visibility of the signal is very high when the fabricated samples present resonances at first and second harmonic frequencies (i.e., 800 and 400 nm, in our case).

Abstract: Chiroptical effects arising in mirror‐symmetric geometrically achiral resonant heterostructures are investigated. It is shown that coalescence of extrinsic chirality, heterogeneous morphology, and substrate‐induced break of symmetry leads to pronounced circular dichroism and circular birefringence. The physics of the involved phenomena is elucidated by studying spin‐splitting in scattering and hybridized dipolar modes of a heterodimer made of gold and silicon nanoparticles of the same shape and size. The work sheds new light on the optical properties of heterogeneous nanostructures and paves the way for designing polarization‐controlled tunable heterogeneous optical elements. [ABSTRACT FROM AUTHOR]

Chiral metamaterials represent a special type of artificial structures that cannot be superposed to their mirror images. Due to the lack of mirror symmetry, cross-coupling between electric and magnetic fields exist in chiral mediums and present unique electromagnetic characters of circular dichroism and optical activity, which provide a new opportunity to tune polarization and realize negative refractive index. Chiral metamaterials have attracted great attentions in recent years and have given rise to a series of applications in polarization manipulation, imaging, chemical and biological detection, and nonlinear optics. Here we review the fundamental theory of chiral media and analyze the construction principles of some typical chiral metamaterials. Then, the progress in extrinsic chiral metamaterials, absorbing chiral metamaterials, and reconfigurable chiral metamaterials are summarized. In the last section, future trends in chiral metamaterials and application in nonlinear optics are introduced. [ABSTRACT FROM AUTHOR]

Plasmonic antennas and planar structures have been undergoing intensive developments in order to control the scattering and absorption of light. One specific class, extrinsic chiral surfaces, that does not possess 2-fold rotational symmetry exhibits strong asymmetric transmission for different circular polarizations under obliquely incident illumination. In this work, we show that the design of those surfaces can be optimized with complex multipolar resonances in order to twist the fluorescence emission from nearby molecules. While this emission is usually dipolar and linearly polarized, the interaction with these resonances twists it into a multipolar radiation pattern with opposite helicity in different directions. The proposed structure maximizes this effect and provides control over the polarization of light. Splitting of left- and right-handed circularly polarized light is experimentally obtained in the backward direction. These results highlight the intricate interplay between the near-field absorption and the far-field scattering of a plasmonic nanostructure and are further used for modifying the emission of incoherent quantum sources. Our finding can potentially lead to the development of polarization- and angle-resolved ultracompact optical devices. [ABSTRACT FROM AUTHOR]

The extrinsic chirality of metasurfaces refers to the chirality produced by the oblique incidence of light, which is observed in achiral meta-structures. Here we propose a new scheme for tunable extrinsic chirality of terahertz metasurface controlled by near-infrared continuous wave. The metasurface is composed of silicon substrate and single-layer metal units, in which the silicon substrate is used as a photosensitive element. The simulated results show that the maximum circular dichroism (CD) in transmission reaches 0.58, when the terahertz wave is incident on the metasurface with an angle of 83 degree. Furthermore, the terahertz CD will decrease under an illumination of optical beam. Simultaneously changing the incidence angle and the power of the pump light, continuous and active control of CD from 0 to 0.58 can be observed. In experiment, the same trend can also be obtained. The metasurface is simple in structure, and it is the first report for the optical tunable extrinsic chirality in terahertz band as far as we know. • It is the first report that the extrinsic chirality has been optical-controlled. • A circular dichroism of 0.58 is achieved via a matasurface with simple structure. • Tuning efficiency of different carrier layer thicknesses is discussed. • Relationship between incident angle and the maximum circular dichroism is found. [ABSTRACT FROM AUTHOR]

Optical circular dichroism (CD) is an important phenomenon in nanophotonics, that addresses top level applications such as circular polarized photon generation in optics, enantiomeric recognition in biophotonics and so on. Chiral nanostructures can lead to high CD, but the fabrication process usually requires a large effort, and extrinsic chiral samples can be produced by simpler techniques. Glancing angle deposition of gold on GaAs nanowires can (NWs) induces a symmetry breaking that leads to an optical CD response that mimics chiral behavior. The GaAs NWs have been fabricated by a self-catalyzed, bottom-up approach, leading to large surfaces and high-quality samples at a relatively low cost. Here, we investigate the second harmonic generation circular dichroism (SHG-CD) signal on GaAs nanowires partially covered with Au. SHG is a nonlinear process of even order, and thus extremely sensitive to symmetry breaking. Therefore, the visibility of the signal is very high when the fabricated samples present resonances at first and second harmonic frequencies (i.e., 800 and 400 nm, in our case). [ABSTRACT FROM AUTHOR]

While most active plasmonic efforts focus on responsive metamaterials to modulate optical response, we present a simple alternative based on applied orientation control that can likely be implemented for many passive plasmonic materials. Passive plasmonic motifs are simpler to prepare but cannot be altered postfabrication. We show that such systems can be easily manipulated through substrate orientation control to generate both active plasmonic and active chiral plasmonic responses. Using gold nanocrescents as our model platform, we demonstrate tuning of optical extinction from -21% to +36% at oblique incidence relative to normal incidence. Variation of substrate orientation in relation to incident polarization is also demonstrated to controllably switch chiroptical handedness ( e.g. , Δ g = ± 0.55). These active plasmonic responses arise from the multipolar character of resonant modes. In particular, we correlate magnetoelectric and dipole-quadrupole polarizabilities with different light-matter orientation-dependence in both near- and far-field localized surface plasmon activity. Additionally, the attribution of far-field optical response to higher-order multipoles highlights the sensitivity offered by these orientation-dependent characterization techniques to probe the influence of localized electromagnetic field gradients on a plasmonic response. The sensitivity afforded by orientation-dependent optical characterization is further observed by the manifestation in both plasmon and chiral plasmon responses of unpredicted structural nanocrescent variance ( e.g. , left- and right-tip asymmetry) not physically resolved through topographical imaging.

For applications seeking to realize on-chip polarization-discriminating nanoantennas, efficient energy conversion from surface waves to far-field radiation is desirable. However, the response of individual nanoantennas to the particular polarization states achievable in surface waves, such as evanescent fields, has not yet been thoroughly investigated. Here, we report the giant modulation of visible light scattering from achiral gold half-rings when switching between evanescent surface wave excitation produced from the total internal reflection of left-handed and right-handed circularly polarized light. The effect is driven by a differing relative phase between the in-plane transverse and longitudinal field oscillations of the evanescent wave depending on the incident light handedness. Because longitudinal field oscillations are not found in free-space excitation, this presents a fundamentally different mechanism for chiroptical responses as traditional mechanisms for circular dichroism only account for purely transversal field oscillations. Although the half-ring scattering modulation is dependent on the wave-vector orientation, an orientation invariant response is also realized in planar chiral nanoantennas composed of 8 half-rings in a rotationally symmetric arrangement, with up to 50% scattering modulation observed at 725 nm. Although both structures are found to produce scattering modulation when switching the handedness of free-space light, the distinct polarization properties of evanescent fields are shown to be strictly required to observe giant scattering modulation. These results ultimately deepen our understanding of the range of possible chiroptical effects in light-matter interactions.

The strong optical chirality arising from certain synthetic metamaterials has important and widespread applications in polarization optics, stereochemistry and spintronics. However, these intrinsically chiral metamaterials are restricted to a complicated three-dimensional (3D) geometry, which leads to significant fabrication challenges, particularly at visible wavelengths. Their planar two-dimensional (2D) counterparts are limited by symmetry considerations to operation at oblique angles (extrinsic chirality) and possess significantly weaker chiro-optical responses close to normal incidence. Here, we address the challenge of realizing strong intrinsic chirality from thin, planar dielectric nanostructures. Most notably, we experimentally achieve near-unity circular dichroism with ~90% of the light with the chosen helicity being transmitted at a wavelength of 540 nm. This is the highest value demonstrated to date for any geometry in the visible spectrum. We interpret this result within the charge-current multipole expansion framework and show that the excitation of higher-order multipoles is responsible for the giant circular dichroism. These experimental results enable the realization of high-performance miniaturized chiro-optical components in a scalable manner at optical frequencies., Competing Interests: The authors declare no conflict of interest.

Chiral metamaterials represent a special type of artificial structures that cannot be superposed to their mirror images. Due to the lack of mirror symmetry, cross-coupling between electric and magnetic fields exist in chiral mediums and present unique electromagnetic characters of circular dichroism and optical activity, which provide a new opportunity to tune polarization and realize negative refractive index. Chiral metamaterials have attracted great attentions in recent years and have given rise to a series of applications in polarization manipulation, imaging, chemical and biological detection, and nonlinear optics. Here we review the fundamental theory of chiral media and analyze the construction principles of some typical chiral metamaterials. Then, the progress in extrinsic chiral metamaterials, absorbing chiral metamaterials, and reconfigurable chiral metamaterials are summarized. In the last section, future trends in chiral metamaterials and application in nonlinear optics are introduced., Competing Interests: The authors declear that there is no conflict of interest.

Plasmonic antennas and planar structures have been undergoing intensive developments in order to control the scattering and absorption of light. One specific class, extrinsic chiral surfaces, that does not possess 2-fold rotational symmetry exhibits strong asymmetric transmission for different circular polarizations under obliquely incident illumination. In this work, we show that the design of those surfaces can be optimized with complex multipolar resonances in order to twist the fluorescence emission from nearby molecules. While this emission is usually dipolar and linearly polarized, the interaction with these resonances twists it into a multipolar radiation pattern with opposite helicity in different directions. The proposed structure maximizes this effect and provides control over the polarization of light. Splitting of left- and right-handed circularly polarized light is experimentally obtained in the backward direction. These results highlight the intricate interplay between the near-field absorption and the far-field scattering of a plasmonic nanostructure and are further used for modifying the emission of incoherent quantum sources. Our finding can potentially lead to the development of polarization- and angle-resolved ultracompact optical devices.