Photonic architectures for synthetic chiral light-driven chiral sensing

Abstract

Molecular chirality gives rise to left- and right-handed enantiomers whose balance underpins biochemical function. Deviations from this enantiomeric excess are promising biomarkers of disease. Despite its importance, rapid and sensitive detection of enantiomeric excess in trace amounts of small chiral molecules remains an outstanding challenge. Synthetic chiral light introduces new opportunities for chiroptical spectroscopy, with the potential to enhance light-matter interactions by several orders of magnitude. Here we propose a new class of photonic architectures for synthetic chiral light, in which photonic structures generate, guide and optimize chiral light-matter interactions. As a first realization, we show that hollow dielectric waveguides support phase-matched propagation of multicolor fields enabling coherent accumulation of the enantio-sensitive nonlinear response over centimeter-scale distances. By combining microscopic quantum-response simulations with Maxwell's equations, we predict that incident pulse energies of around 1 uJ produce hundreds of picojoules of third-harmonic emission from only picomole quantities of carvone gas at 50 mbar over just 2 cm of propagation, with enantio-sensitive contrast approaching 5%. Phase-resolved Fourier analysis isolates a background-free chiral signal exhibiting the maximum possible dichroism of 200%. Beyond efficient chiral sensing, photonic architectures for synthetic chiral light establish a scalable platform for integrated nonlinear chiral spectroscopy, molecular fingerprinting based on ultrafast electron dynamics, and topologically robust chiroptical observables.