Core-Valence Attosecond Transient Absorption Spectroscopy of Polyatomic Molecules.

ABSTRACT

Tracing ultrafast processes induced by interaction of light with matter is often very challenging. In molecular systems, the initially created electronic coherence becomes damped by the slow nuclear rearrangement on a femtosecond timescale which makes real-time observations of electron dynamics in molecules particularly difficult. In this work, we report an extension of the theory underlying the attosecond transient absorption spectroscopy (ATAS) for the case of molecules, including a full account for the coupled electron-nuclear dynamics in the initially created wave packet, and apply it to probe the oscillations of the positive charge created after outer-valence ionization of the propiolic acid molecule. By taking advantage of element-specific core-to-valence transitions induced by x-ray radiation, we show that the resolution of ATAS makes it possible to trace the dynamics of electron density with atomic spatial resolution.