Double Photodetachment of F¯∙H 2 O: Experimental and Theoretical Studies of [F∙H 2 O] .

Double photodetachment of the cluster F‾•H2 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 wavefunction, shed light on the Franck-Condon region and ab initio molecular dynamics (AIMD) simulations also performed using EOM-CC methods reveal the fragmentation dynamics in time on the lowest lying singlet and triplet states of [F•H2 O]+ . The simulations show the formation of H2 O+ + F, which is the predominant experimentally observed product channel. Suggestions are proposed for the formation mechanisms of the minor products, e.g. the very interesting H2 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.