Double photodetachment of the cluster F - ·H 2 O in a strong laser field is explored in a combined experimental-theoretical study. Products are observed experimentally by coincidence photofragment imaging following double ionization by intense laser pulses. Theoretically, equation of motion coupled cluster calculations (EOM-CC), suitable for modeling strong correlation effects in the electronic wave function, shed light on the Franck-Condon region, and ab initio molecular dynamics simulations also performed using EOM-CC methods reveal the fragmentation dynamics in time on the lowest-lying singlet and triplet states of [F·H 2 O] + . The simulations show the formation of H 2 O + + F, which is the predominant experimentally observed product channel. Suggestions are proposed for the formation mechanisms of the minor products, for example, the very interesting H 2 F + , which involves significant geometrical rearrangement. Analysis of the results suggests interesting future directions for the exploration of photodetachment of anionic clusters in an intense laser field.
Bibliographical noteFunding Information:
US-Israel BSF grant #2014701, Israel Science Foundation grant #1369/17, and Zuckerman STEM Leadership Fellowship are acknowledged. The authors also thank Professor Anna Krylov for her helpful comments on EOM methods.
© 2018 American Chemical Society.