Strong chiral dichroism and enantiopurification in above-threshold ionization with locally chiral light

We derive here a new highly selective photoelectron-based chirality-sensing technique that utilizes 'locally-chiral' laser pulses. show this approach results in strong chiral discrimination, where the standard forwards/backwards asymmetry of photoelectron circular dichroism (PECD) is lifted. The resulting much larger and more robust than conventional PECD, found all hemispheres, not symmetric or antisymmetric with respect to any symmetry operator. Remarkably, CD up 10% survives angularly-integrated above-threshold ionization (ATI) spectra, 5% total rates. demonstrate these through ab-initio calculations molecules Bromochlorofluoromethane, Limonene, Fenchone, Camphor. also explore parameter-space locally-chiral field observed strongly correlated degree chirality light, validating it as measure for chiral-interaction strengths. Our pave way probing ultrafast ATI, can potentially lead all-optical enantio-separation, motivate use light enhancing spectroscopies.