Phase-matched locally chiral light for global control of chiral light-matter interaction

Abstract: 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.