A new path towards reconstructing real-space geometries of polyatomic molecules undergoing strong field laser-induced Coulomb explosion

Abstract The connection between the initial structure and final momenta of ionic fragments from the Coulomb explosion of a multiatomic molecule is investigated experimentally and theoretically for OCS. We show for the first time that an approach using time-dependent density functional theory (TDDFT) is able to rigorously model the ionization dynamics of a small molecule in the tunneling regime, reproducing the energy release and the Newton plot momentum patterns of an experiment in which OCS is ionized to the 6+ charge state using 7 fs laser pulses of 800 nm. The result suggests a pathway to unprecedented understanding of the behavior of molecules, during strong field multiple ionization and the possibility of precision imaging of real-space molecular geometries, using tabletop lasers.