The differential response of chiral molecules to incident left-and right-handed circularly polarized light is used for sensing the handedness of molecules. Currently, significant effort is directed toward enhancing weak differential signals from the molecules, with the goal of extending the capabilities of chiral spectrometers to lower molecular concentrations or small analyte volumes. Previously, optical cavities for enhancing vibrational circular dichroism have been introduced. Their enhancements are mediated by helicity-preserving cavity modes which maintain the handedness of light due to their degenerate TE and TM components. In this article, we simplify the design of the cavity and numerically compare it with the previous one using an improved model for the response of chiral molecules. We use parameters of molecular resonances to show that the cavities are capable of bringing the vibrational circular dichroism signal over the detection threshold of typical spectrometers for concentrations that are one to three orders of magnitude smaller than those needed without the cavities, for a fixed analyte volume. Frequency resolutions of current spectrometers result in enhancements of more than one order (two orders) of magnitude for the new (previous) design. With improved frequency resolution, the new design achieves enhancements of three orders of magnitude. We show that the TE/ TM degeneracy in perfectly helicity-preserving modes is lifted by factors that are inherent to the cavities. More surprisingly, this degeneracy is also lifted by the molecules themselves due to their lack of electromagnetic duality symmetry, that is, due to the partial change of helicity during the light-molecule interactions.
Being able to sense and distinguish the handedness of chiral molecules is crucial for many applications in the life sciences. Here, we explore by theoretical and computational means the ability of achiral and helicity preserving photonic nanostructures to enhance the optical rotation, i.e., the polarization rotation of elliptically polarized light while traversing a solution of chiral molecules. Starting from a helicity preserving isolated dielectric cylinder, we assemble an array thereof, which enhances the optical rotation power by a factor of four, being limited by the inability to enhance the helicity density beyond the near fields attached to the array. To overcome this limitation, we study cavities composed of two arrays of cylinders with the solution of molecules in between. Such cavities enhance the optical rotation power by a factor as large as 270. Our work complements previous research that concentrated on enhancing circular dichroism with similar structures. Measuring and enhancing circular dichroism as well as optical rotation provides more complete information about the molecules under investigation.
The differential response of chiral molecules to incident left-and right-handed circularly polarized light is used for sensing the handedness of molecules. Currently, significant effort is directed toward enhancing weak differential signals from the molecules, with the goal of extending the capabilities of chiral spectrometers to lower molecular concentrations or small analyte volumes. Previously, optical cavities for enhancing vibrational circular dichroism have been introduced. Their enhancements are mediated by helicity-preserving cavity modes which maintain the handedness of light due to their degenerate TE and TM components. In this article, we simplify the design of the cavity and numerically compare it with the previous one using an improved model for the response of chiral molecules. We use parameters of molecular resonances to show that the cavities are capable of bringing the vibrational circular dichroism signal over the detection threshold of typical spectrometers for concentrations that are one to three orders of magnitude smaller than those needed without the cavities, for a fixed analyte volume. Frequency resolutions of current spectrometers result in enhancements of more than one order (two orders) of magnitude for the new (previous) design. With improved frequency resolution, the new design achieves enhancements of three orders of magnitude. We show that the TE/ TM degeneracy in perfectly helicity-preserving modes is lifted by factors that are inherent to the cavities. More surprisingly, this degeneracy is also lifted by the molecules themselves due to their lack of electromagnetic duality symmetry, that is, due to the partial change of helicity during the light-molecule interactions.
A theoretical paper based on chiral micropolar effective‐medium theory suggested the possibility of unusual roton‐like acoustical‐phonon dispersion relations in 3D elastic materials. Here, as a first novelty, the corresponding inverse problem is solved, that is, a specific 3D chiral elastic metamaterial structure is designed, the behavior of which follows this effective‐medium description. The metamaterial structure is based on a simple‐cubic lattice of cubes, each of which not only has three translational but also three rotational degrees of freedom. The additional rotational degrees of freedom are crucial within micropolar elasticity. The cubes and their degrees of freedom are coupled by a chiral network of slender rods. As a second novelty, this complex metamaterial is manufactured in polymer form by 3D laser printing and its behavior is characterized experimentally by phonon‐band‐structure measurements. The results of these measurements, microstructure finite‐element calculations, and solutions of micropolar effective‐medium theory are in good agreement. The roton‐like dispersion behavior of the lowest phonon branch results from two aspects. First, chirality splits the transverse acoustical branches as well as the transverse optical branches. Second, chirality leads to an ultrastrong coupling and hybridization of chiral acoustical and optical phonons at finite wavevectors.
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