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Register a new userDynamically reversible and strong circular dichroism based on Babinet-invertible chiral metasurfaces
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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.
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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
Recently, we proposed a metasurface design for chiral sensing that (i) results in enhanced chiroptical signals by more than two orders of magnitude for ultrathin, subwavelength, chiral samples over a uniform and accessible area, (ii) allows for complete measurements of the total chirality (magnitude and sign of both its real and imaginary part), and (iii) offers the possibility for a crucial signal reversal (excitation with reversed polarization) that enables chirality measurements in an absolute manner, i.e., without the need for sample removal. Our design is based on the anisotropic response of the metasurface, rather than the superchirality of the generated near-fields, as in most contemporary nanophotonic-based chiral sensing approaches. Here, we derive analytically, and verify numerically, simple formulas that provide insight to the sensing mechanism and explain how anisotropic metasurfaces, in general, offer additional degrees of freedom with respect to their isotropic counterparts. We provide a detailed discussion of the key functionalities and benefits of our proposed design and we demonstrate practical measurement schemes for the unambiguous determination of an unknown chirality. Last, we provide the design principles towards broadband operation - from near-infrared to near-ultraviolet frequencies - opening the way for highly sensitive nanoscale chiroptical spectroscopy.
In this work we present a new mechanism for designing phase-gradient metasurfaces (PGMs) to control an electromagnetic wavefront with high efficiency. Specifically, we design a transmission-type PGM formed by a periodic subwavelength metallic slit array filled with identical dielectrics of different heights. It is found that when Fabry-Perot (FP) resonances occur locally inside the dielectric regions, in addition to the common phenomenon of complete transmission, the transmitted phase differences between two adjacent slits are exactly the same, being a non-zero constant. These local FP resonances ensure total phase shift across a supercell that can fully cover the range of 0 to 2Pi, satisfying the design requirements of PGMs. More studies reveal that due to local FP resonances, there is a one-to-one correspondence between the phase difference and the permittivity of the filled dielectric. A similar approach can be extended to the reflection-type case and other wavefront transformation, creating new opportunities for wave manipulation.
Chirality is ubiquitous in nature and fundamental in science, from particle physics to metamaterials.The most established technique of chiral discrimination - photoabsorption circular dichroism - relies on the magnetic properties of a chiral medium and yields an extremely weak chiral response. We propose and demonstrate a new, orders of magnitude more sensitive type of circular dichroism in neutral molecules: photoexitation circular dichroism. It does not rely on weak magnetic effects, but takes advantage of the coherent helical motion of bound electrons excited by ultrashort circularly polarized light. It results in an ultrafast chiral response and the efficient excitation of a macroscopic chiral density in an initially isotropic ensemble of randomly oriented chiral molecules. We probe this excitation without the aid of further chiral interactions using linearly polarized laser pulses. Our time-resolved study of vibronic chiral dynamics opens a way to the efficient initiation, control and monitoring of chiral chemical change in neutral molecules at the level of electrons.
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.
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