Attosecond coherent control of oxygen dissociation by XUV-IR laser fields using three-dimensional momentum imaging

Author(s): Ranitovic, P; Sturm, FP; Tong, XM; Wright, TW; Ray, D; Zalyubovskya, I; Shivaram, N; Belkacem, A; Slaughter, DS; Weber, T | Abstract: © 2018 American Physical Society. We have performed ultrafast three-dimensional ion momentum imaging spectroscopy on the dissociative single ionization of oxygen molecules using attosecond pulse trains with a broad energy spectrum of 5-30 eV. High-resolution momentum imaging allows clear identification of vibrational structures corresponding to the predissociation of highly excited cationic states. By adding a pump infrared field that is synchronized with and polarized orthogonally to the XUV pulse train, and an additional probe IR field, we demonstrate how the yield of O+ ions can be steered between different dissociation channels by coherently controlling the coupling between multiple O2+∗ electronic states on an attosecond time scale. Time-dependent calculations in a single active electron approximation allow a qualitative analysis of ion yields for two orientations of the molecular axis.