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Register a new userFluorescence-Detected Circular Dichroism of a Chiral Molecular Monolayer with Dielectric Metasurfaces
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Strong enhancement of molecular circular dichroism has the potential to enable efficient asymmetric photolysis, a method of chiral separation that has conventionally been impeded by insufficient yield and low enantiomeric excess. Here, we study experimentally how predicted enhancements in optical chirality density near resonant silicon nanodisks boost circular dichroism. We use fluorescence-detected circular dichroism spectroscopy to measure indirectly the differential absorption of circularly polarized light by a monolayer of optically active molecules functionalized to silicon nanodisk arrays. Importantly, the molecules and nanodisk antennas have spectrally-coincident resonances, and our fluorescence technique allows us to deconvolute absorption in the nanodisks from the molecules. We find that enhanced fluorescence-detected circular dichroism signals depend on nanophotonic resonances in good agreement with simulated differential absorption and optical chirality density, while no signal is detected from molecules adsorbed on featureless silicon surfaces. These results verify the potential of nanophotonic platforms to be used for asymmetric photolysis with lower energy requirements
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We propose a Babinet-invertible chiral metasurface for achieving dynamically reversible and strong circular dichroism (CD). The proposed metasurface is composed of VO$_2$-metal hybrid structure, and when VO$_2$ transits between the dielectric state and the metallic state, the metasurface unit cell switches between complementary structures that are designed according to the Babinet principle. This leads to a large and reversible CD tuning range between $pm 0.5$ at 0.97~THz, which is larger than the literature. We attribute the CD effect to extrinsic chirality of the proposed metasurface. We envision that the Babinet-invertible chiral metasurface proposed here will advance the engineering of active and tunable chiro-optical devices and promote their applications.
Electromagnetic fields coupled with mechanical degrees of freedom have recently shown exceptional and innovative applications, ultimately leading to mesoscopic optomechanical devices operating in the quantum regime of motion. Simultaneously, micromechanical elements have provided new ways to enhance and manipulate the optical properties of passive photonic elements. Following this concept, in this article we show how combining a chiral metasurface with a GaAs suspended micromembrane can offer new scenarios for controlling the polarization state of near-infrared light beams. Starting from the uncommon properties of chiral metasurface to statically realize target polarization states and circular and linear dichroism, we report mechanically induced, ~300 kHz polarization modulation, which favorably compares, in terms of speed, with liquid-crystals commercial devices. Moreover, we demonstrate how the mechanical resonance can be non-trivially affected by the input light polarization (and chiral state) via a thermoelastic effect triggered by intracavity photons. This work inaugurates the field of Polarization Optomechanics, which could pave the way to fast polarimetric devices, polarization modulators and dynamically tunable chiral state generators and detectors, as well as giving access to new form of polarization nonlinearities and control.
In the close vicinity of a chiral nanostructure, the circular dichroism of a biomolecule could be greatly enhanced, due to the interaction with the local superchiral fields. Modest enhancement of optical activity using a planar metamaterial, with some chiral properties, and achiral nanoparticles has been previously reported. A more substantial chirality enhancement can be achieved in the local filed of a chiral nanostructure with a three-dimensional arrangement. Using an embossed chiral nanostructure designed for chiroptical sensing, we measure the circular dichroism spectra of two biomolecules, Chlorophylls A and B, at the molecular level, using a simple polarization resolved reflection measurement. This experiment is the first realization of the on-resonance surface-enhanced circular dichroism, achieved by matching the chiral resonances of a strongly chiral metamaterial with that of a chiral molecule, resulting in an unprecedentedly large differential CD spectrum from a monolayer of a chiral 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 is determined by the chiral localized plasmonic resonances.
We use numerical simulations to demonstrate third-harmonic generation with near-unity nonlinear circular dichroism (CD) and high conversion efficiency ($ 10^{-2} text{W}^{-2}$) in asymmetric Si-on-SiO$_2$ metasurfaces. The working principle relies on the selective excitation of a quasi-bound state in the continuum, characterized by a very high ($>10^5$) quality-factor. By tuning multi-mode interference with the variation of the metasurface geometrical parameters, we show the possibility of independent control of linear CD and nonlinear CD. Our results pave the way for the development of all-dielectric metasurfaces for nonlinear chiro-optical devices with high conversion efficiency.
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