Size Effects in the Strong-Field Ionization and Dissociation Dynamics of (H$_2$O)$_n$ (n=1-4)

Abstract

The size-dependent strong-field ionization and dissociation dynamics of (H$_2$O)$_n$ (n=1-4) are investigated using real-time time-dependent density functional theory (RT-TDDFT) coupled to Ehrenfest molecular dynamics under a common few-cycle near-infrared laser pulse. It is found that the net ionization per monomer varies only weakly on cluster size, whereas the protonic and oxygen response is changed much more strongly once the cluster size grows beyond the dimer. In particular, H-ejection activity is observed to rise sharply from the dimer to the trimer/tetramer regime, while stable H-transfer is essentially absent in the dimer under the present criterion but becomes substantial in the trimer and is further amplified in the tetramer. Through timing analyses, it is shown that the dimer exhibits a weak and temporally broad response, whereas the larger clusters display a much stronger early-time protonic response concentrated within and immediately after the laser pulse window. By endpoint oxygen statistics, a systematic increase in dissociation propensity with cluster size is likewise shown. For a clean subset of direct two-body dimer breakup trajectories, the asymptotic kinetic energy release is estimated to be 4.47 $\pm$ 1.03 eV, in reasonably good agreement with the experimental value for the unprotonated two-body Coulomb-explosion channel. Overall, it is shown by the results that increasing water-cluster size primarily reshapes the strong-field response through proton-mediated and topology-level nuclear dynamics rather than through a large change in net ionization alone.