Abstract:

Molecular ordering at interfaces activates chiral-specific light-matter interactions that disappear in isotropic systems. Chiral-specific responses are often fully electric dipole-allowed, rivaling in magnitude their achiral counterparts. The unique symmetry properties tied to spectroscopy of chiral interfaces open up a host of novel spectroscopic effects with impacts spanning biological analysis to quantum computing. Our early work on second harmonic and sum-frequency spectroscopy of chiral interfaces has served as a foundation for development of instrumentation for selective nonlinear optical imaging of homochiral crystals, enabling new strategies in macromolecular crystallography and pharmaceutical formulations design. Ongoing efforts seek to expand on our early predictions of chiral-specific and interface-specific four-wave mixing, using that framework to interpret large chiral-specific spectroscopic effects in fluorescence and absorbance spectroscopy of oriented assemblies. Specifically, we aim to develop new experimental strategies for acquiring and interpreting spectroscopic measurements of chiral interfaces, targeting a host of potentially impactful downstream applications.