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