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Chiral plasmonic nanostructures enable ≤pg detection and characterization of biomaterials. The sensing capabilities are associated with the chiral asymmetry of the near fields, which locally can be greater than equivalent circularly polarized light, a property referred to as superchirality. However, sensing abilities do not simply scale with the magnitude of superchirality. We show that chiral molecular sensing is correlated to the thickness of a nanostructure. This observation is reconciled with a previously unconsidered interference mechanism for the sensing phenomenon. It involves the “dissipation” of optical chirality into chiral material currents through the interference of fields generated by two spatially separated chiral modes. The presence of a chiral dielectric causes an asymmetric change in the phase difference, resulting in asymmetric changes to chiroptical properties. Thus, designing a chiral plasmonic sensor requires engineering a substrate that can sustain both superchiral fields and an interference effect.

Roles of Superchirality and Interference in Chiral Plasmonic Biodetection