Quantum contributions to Coulomb-explosion imaging revealed by trajectory-surface-hopping molecular dynamics

We compare trajectory-surface-hopping (TSH) calculations of the dissociation of quadruply charged formaldehyde molecules with basic classical calculations assuming Coulomb repulsion between singly charged atoms. The TSH calculations show very different dissociation dynamics from the classical Coulomb calculations, illustrating that Coulomb repulsion between point charges does not accurately describe the dissociation dynamics. By comparing the calculations with covariance measurements, we see much better agreement between the experiments and the TSH calculations, and evidence for the production of multiple electronic states of the tetracation via strong-field ionization.