Disentangling Strong-Field Multielectron Dynamics with Angular Streaking

The study into the interaction between a strong laser field and atoms/molecules has led to significant advances in developing spectroscopic tools in the attosecond time-domain and methods for controlling chemical reactions. There has been great interest in understanding the complex electronic and nuclear dynamics of molecules in strong laser fields. However, it is still a formidable challenge to fully model such dynamics. Conventional experimental tools such as photoelectron spectroscopy encounter difficulties in revealing the involved states because the electron spectra are largely dictated by the property of the laser field. Here, with strong field angular streaking technique, we measure the angle-dependent ionization yields that directly reflect the symmetry of the ionizing orbitals of methyl iodide and thus reveal the ionization/dissociation dynamics. Moreover, kinematically complete measurements of momentum vectors of all fragments in dissociative double ionization processes allow access to electron-momentum correlations that reveal correlated multielectron dynamics.