Tilting light's polarization plane to spatially separate the ultrafast nonlinear response of chiral molecules

Distinguishing between the left- and right-handed versions of a chiral molecule (enantiomers) is vital, but also inherently difficult. Traditional optical methods using elliptically/circularly polarized light rely on linear effects which arise beyond the electric-dipole approximation, posing major limitations for ultrafast spectroscopy. Here we show how to turn an ultrashort elliptical pulse into an efficient chiro-optical tool: by tilting its polarization plane towards its propagation direction. This forward tilt can be achieved by focusing the beam tightly, creating structured light which exhibits a nontrivial polarization pattern in space. Using state-of-the-art computational modelling, we show that our structured field realizes a near-field interferometer for efficient chiral recognition that separates the nonlinear optical response of left- and right-handed molecules in space. Our work provides a simple, yet highly efficient, way of spatially structuring the polarization of light to image molecular chirality, with extreme enantio-efficiency and on ultrafast time scales.