Fluorescence-Detected Circular Dichroism of a Chiral Molecular Monolayer with Dielectric Metasurfaces

TL;DR

This study demonstrates how dielectric metasurfaces can significantly enhance molecular circular dichroism signals, enabling more efficient chiral photolysis through nanophotonic resonance effects.

Contribution

The paper experimentally shows fluorescence-detected circular dichroism enhancement using silicon nanodisks with coincident resonances, verified by simulations and absent on flat silicon.

Findings

Enhanced CD signals depend on nanophotonic resonances

No CD signal from molecules on flat silicon surfaces

Potential for lower-energy asymmetric photolysis

Abstract

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