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Enantiospecific optical enhancement of chiral sensing and separation with dielectric metasurfaces

AuthorsSolomon, Michelle L.; Hu, Jack; Lawrence, Mark; García-Etxarri, Aitzol ; Dionne, Jennifer
Dielectric nanoparticles
Enantiomer separation
Kerker conditions
Mie resonances
Issue Date2019
PublisherAmerican Chemical Society
CitationACS Photonics 6(1): 43-49 (2019)
AbstractCircularly polarized light (CPL) exhibits an enantioselective interaction with chiral molecules, providing a pathway toward all-optical chiral resolution. High index dielectric nanoparticles have been shown to enhance this relationship, but with a spatially varying sign (or enantiospecificity) that yields a near zero spatially averaged enhancement. Using full field electromagnetic simulations, we design metasurfaces consisting of high index dielectric disks that provide large-volume, uniform-sign enhancements in both the optical density of chirality, C (the figure of merit for sensing and spectroscopy), and Kuhn’s dissymmetry factor, g (the figure of merit for separation). By varying disk radius, we achieve local enhancements in C and g up to 138-fold and 15-fold, respectively, as well as volumetric enhancements of 30-fold and 4.2-fold. The uniform-sign enhancements in C occur near the first Kerker condition, where overlapping electric and magnetic modes maximize field strength and preserve the π/2 phase lag between the electric and magnetic fields of CPL; in contrast, uniform-sign enhancements in g occur with spectrally separated modes, where fields and phase remain optimal without reduced molecular absorption. Using first-order kinetics of the molecule thiocamphor, we show how this optically enantiopure metasurface could enable 20% enantiomeric excesses with a >2000-fold increase in yield for a photoionization reaction compared to CPL alone.
Publisher version (URL)https://doi.org/10.1021/acsphotonics.8b01365
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