  Locally chiral light is an emerging tool for probing and controlling
molecular chirality. It can generate large and freely adjustable
enantioselectivities in purely electric-dipole effects, offering its major
advantages over traditional chiral light. However, the existing types of
locally chiral light are phase-mismatched, and thus the global efficiencies are
greatly reduced compared with the maximum single-point efficiencies or even
vanish. Here, we propose a scheme to generate phase-matched locally chiral
light. To confirm this advantage, we numerically show the robust highly
efficient global control of enantiospecific electronic state transfer of
methyloxirane at nanoseconds. Our work potentially constitutes the starting
point for developing more efficient chiroptical techniques for the studies of
chiral molecules.

Optics