Abstract
Chiral discrimination, a problem of vital importance, has recently become an emerging frontier in ultrafast physics, with remarkable progress achieved in multiphoton and strong-field regimes. Rydberg excitations, unavoidable in the strong-field regime and intentional for few-photon processes, arise in all these approaches. Here, we show how to harness this ubiquitous feature by introducing a new phenomenon, enantiosensitive free-induction decay, steered by a tricolor chiral field at a gentle intensity, structured in space and time. We demonstrate theoretically that an excited chiral molecule accumulates an enantiosensitive phase due to perturbative interactions with the tricolor chiral field, resulting in a spatial phase gradient steering the free-induction decay in opposite directions for opposite enantiomers. Our work introduces a general, extremely sensitive, all-optical enantiosensitive detection technique that avoids strong fields and takes full advantage of recent advances in structuring light.