We introduce an ultrafast all-optical approach for efficient chiral recognition which relies on the interference between two low-order nonlinear processes which are ubiquitous in nonlinear optics: sum-frequency generation
and third-harmonic generation. In contrast to traditional sum-frequency generation, our approach encodes the medium’s handedness in the intensity of the
emitted harmonic signal, rather than in its phase, and it enables full control
over the enantiosensitive response. We show how, by sculpting the sub-opticalcycle oscillations of the driving laser field, we can force one molecular enantiomer to emit bright light while its mirror twin remains dark, thus reaching
the ultimate efficiency limit of chiral sensitivity via low-order nonlinear lightmatter interactions. Our work paves the way for ultrafast and highly efficient
imaging and control of the chiral electronic clouds of chiral molecules using
lasers with moderate intensities, in all states of matter: from gases to liquids
to solids, with molecular specificity and on ultrafast timescales.