Ultrafast molecular chirality: twisting light to twist electrons on ultrafast time scale

Chiral molecules are characterized by specific stereo arrangements of their nuclei underlying their key function in chemistry and biology. Yet, little is known about chiral molecular interactions at the level of electrons, occurring on the ultrafast time scale. Developing extremely efficient enantio-sensitive ultrafast all-optical approaches to track electronic dynamics is an important unsolved challenge. We aim to address it in ULISSES a multidisciplinary project at the interface of physical chemistry, strong-field physics, ultrafast and nonlinear optics.We plan to take advantage of the chiral electron currents, which arise naturally in chiral molecules interacting with sufficiently intense ultrafast light. The chiral nature of these currents is dictated by the molecule itself. We will structure laser polarization in space and time, endowing light with local chiral and global topological properties, to control these electron currents, enabling new, orders of magnitude more efficient, enantio-sensitive all-optical effects, gaining access to the ultrafast electron dynamics and physical mechanisms underlying the chiral function. We will also develop a framework for describing geometrical magnetism, generated by the electron currents in chiral molecules, and introduce a new class of enantio-sensitive phenomena enabled by these geometric concepts.We aim to establish: 1) novel, highly efficient, all-optical ways of enantio-discrimination, 2) enantio-resolved movies of chiral electronic dynamics, 3) chiral topological light a new tool for chiral interactions, and 4) bridges between light-driven electron dynamics in chiral gases and topological effects in solids. ULISSES will dramatically expand fundamental understanding of the dynamical response of chiral systems to light and lay the foundation for innovative applications of all-optical methods to chiral discrimination in low-density samples with extraordinary sensitivity and molecular specificity.