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Register a new userAchiral, Helicity Preserving, and Resonant Structures for Enhanced Sensing of Chiral Molecules
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Added by
Ivan Fernandez-Corbaton
Publication date
2018
fields
Physics
and research's language is
English
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We derive a set of design requirements that lead to structures suitable for molecular circular dichroism (CD) enhancement. Achirality of the structure and two suitably selected sequentially incident beams of opposite helicity ensures that the CD signal only depends on the chiral absorption properties of the molecules, and not on the achiral ones. Under this condition, a helicity preserving structure, which prevents the coupling of the two polarization handednesses, maximizes the enhancement of the CD signal for a given ability of the structure to enhance the field. When the achirality and helicity preservation requirements are met, the enhancement of the CD signal is directly related to the enhancement of the field. Next, we design an exemplary structure following the requirements. The considered system is a planar array of silicon cylinders under normally incident plane-wave illumination. Full-wave numerical calculations show that the enhancement of the transmission CD signal is between 6.5 and 3.75 for interaction lengths between 1.25 and 3 times the height of the cylinders.
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Researchers routinely sense molecules by their infrared vibrational fingerprint absorption resonances. In addition, the dominant handedness of chiral molecules can be detected by circular dichroism (CD), the normalized difference between their optical response to incident left- and right- handed circularly polarized light. Here, we introduce a cavity composed of two parallel arrays of helicity-preserving silicon disks that allows to enhance the CD signal by more than two orders of magnitude for a given molecule concentration and given thickness of the cell containing the molecules. The underlying principle is first-order diffraction into helicity-preserving modes with large transverse momentum and long lifetimes. In sharp contrast, in a conventional Fabry-Perot cavity, each reflection flips the handedness of light, leading to large intensity enhancements inside the cavity, yet to smaller CD signals than without the cavity.
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.
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 towards 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.
Although it is commonly believed that all the volumetric optical force laws should lead to the same total optical force for chiral and achiral objects, this idea has been invalidated in some recent works by investigating several previous experiments involving material background. To identify the exact reason of such significant disagreement, we inspect two tractor beam and one lateral force experiments on using distinct stress tensors (STs). To solve the problems of total force, we propose two consistency conditions of time averaged forces. We demonstrate that exactly at the boundary of an object, the difference of the consistent external Minkowski ST and internal ST of Chu (and Einstein-Laub) is found in agreement with the surface force yielded by Chu (and Einstein-Laub) force only when the background is air rather than a material. We identify this as one of the main reasons (among few other identified reasons) of the disagreements observed for real experiments. Finally, based on the proposed consistency conditions, we demonstrate that: by modifying the Einstein-Laub or Chu formulation, time-averaged STs and volume forces are obtainable those can overcome the aforementioned inconsistencies of real experiments for both chiral and achiral Mie objects embedded in even complex material backgrounds.
Chirality refers to a geometric phenomenon in which objects are not superimposable on their mirror image. Structures made of nano-scale chiral elements can display chiroptical effects, such as dichroism for left- and right- handed circularly polarized light, which makes them of high interest for applications ranging from quantum information processing and quantum optics to circular dichroism spectroscopy and molecular recognition. At the same time, strong effects have been challenging to achieve even in synthetic optical media and chiroptical effects for light with normal incidence has been speculated to be prohibited in lossless, thin, quasi-two-dimensional structures. Here, we report on our experimental realization of a giant chiroptical effect in a thin monolithic photonic crystal mirror. Unlike conventional mirrors, our structure selectively reflects only one spin state of light, while preserving its handedness, with a near unity level of circular dichroism. The operational principle of the photonic-crystal mirror relies on Guided Mode Resonance (GMR) with simultaneous excitation of leaky TE and TM Bloch modes in the photonic crystal slab. Such modes are not reliant on the suppression of their radiative losses through the long-range destructive interference and even small areas of the photonic-crystal exhibit robust circular dichroism. Despite its simplicity, the mirror strongly surpasses the performance of earlier reported structures and, contrary to a prevailed notion, demonstrates that near unity reflectivity contrast for the opposite helicities is achievable in a quasi-two-dimensional structure.
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