Ultrafast Imaging of Molecular Chirality with Photoelectron Vortices

Ultrafast imaging of molecular chirality is a key step toward the dream of imaging and interpreting electronic dynamics in complex and biologically relevant molecules. Here, we propose a new ultrafast chiral phenomenon exploiting recent advances in electron optics allowing access to the orbital angular momentum of free electrons. We show that strong-field ionization of a chiral target with a few-cycle linearly polarized 800 nm laser pulse yields photoelectron vortices, whose chirality reveals that of the target, and we discuss the mechanism underlying this phenomenon. Our Letter opens new perspectives in recollision-based chiral imaging.