Two-Dimensional Control of Rydberg Fragment Emission in Dissociative Frustrated Ionization of Oxygen

Advances in producing tailored ultrashort laser pulses have enabled the generation and control of molecular dissociative Rydberg excitation along the polarization axis of the laser field. Here, we exploit the orthogonally polarized two-color femtosecond laser fields and achieve an unprecedented two-dimensional control of Rydberg fragment emission in the dissociative frustrated single ionization of oxygen. The Rydberg fragments are collected over the 4π solid angle, whose momentum distribution is manifested in a characteristic four-lobe pattern. Through precise scanning of the relative phase of the orthogonal two-color laser fields, we demonstrate control over asymmetric directional emission of the Rydberg fragments. Our experimental findings are well supported by classical trajectory Monte Carlo simulations, which suggest an efficient emission control achieved through the manipulation of charge localization upon ionization.