Ultrafast chiral imaging with photoelectron vortices

Molecular chirality plays a decisive role in determining the outcome of molecular reactions, plays a fundamental role in biological systems, and has an immense importance for the chemical industry. The investigation of the interaction between intense short pulses of light and chiral matter has unveiled an array of highly enantio-sensitive phenomena, among which photoelectron techniques have received much attention. Simultaneously, there is an ongoing effort aimed at generating and characterizing electron vortices – electron waves with a helical phase front carrying orbital angular momentum. Electron vortices are expected to provide fundamentally new ways to image chiral matter but their study has been mostly limited to electron transmission microscopy and their potential for ultrafast imaging remains largely unexplored. Here we provide what is to our knowledge the first example of how to exploit photoelectron vortices for the purposes of ultrafast imaging of molecular chirality. Namely, we predict that an intense, linearly polarized, few-cycle, infrared pulse can project the chirality of the molecule onto the photoelectron vortex resulting from the strong-field ionization event. We support our prediction with accurate TDSE simulations in a model chiral system.