Recent experimental and theoretical work has investigated the double photodetachment of the cluster F-●H2O in an intense laser field to form [F●H2O]+. The products of this double photodetachment were determined to be H2O+, OH+, O+, HF+, and H2F+. The products HF+ and H2F+ require significant geometrical rearrangement of the cluster, indicating surprising and interesting dynamical processes. Characterization of the reaction pathway on the lowest-lying triplet and singlet states via intrinsic reaction coordinate (IRC) analysis and ab initio molecular dynamics (AIMD) simulations was performed. Due to the diradical character of the [F●H2O]+ cluster, the double ionization EOM-CCSD method was chosen for theoretical study of the system. The high degree of correlation and multireference nature of the theory make this method ideal for studying the dynamical processes of this system. Initial studies focused on ground state dynamics and showed that the predominant process is separation of H2O+ and F. Moreover, the initial studies indicate that formation of OH+, O+, HF+, and H2F+ largely occurs with involvement of excited states. Here we present studies of the excited state dynamics of [F●H2O]+ and compare theoretical product yields to experimental values. We furthermore discuss difficulties in treating the high density of electronic states, surface hopping, and future directions.

Excited state dynamics involved in the double photodetachment of F-●H2O in an intense laser field

2019 Spring National Meeting

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