Step-by-step state-selective tracking of fragmentation dynamics of water dications by momentum imaging

Journal Article · 01 September 2022 · Nature Communications

DOI: https://doi.org/10.1038/s41467-022-32836-6 · OSTI ID:1885176

Severt, Travis; Streeter, Zachary L.; Iskandar, Wael; Larsen, Kirk A.; Gatton, Averell; Trabert, Daniel ; Jochim, Bethany; Griffin, Brandon ; Champenois, Elio G.; Brister, Matthew M.; Reedy, Dylan; Call, Demitri; Strom, Richard; Landers, Allen L.; Dörner, Reinhard ; Williams, Joshua B.; Slaughter, Daniel S. ; Lucchese, Robert R. ; Weber, Thorsten ; McCurdy, C. William ; Ben-Itzhak, Itzik

Abstract The double photoionization of a molecule by one photon ejects two electrons and typically creates an unstable dication. Observing the subsequent fragmentation products in coincidence can reveal a surprisingly detailed picture of the dynamics. Determining the time evolution and quantum mechanical states involved leads to deeper understanding of molecular dynamics. Here in a combined experimental and theoretical study, we unambiguously separate the sequential breakup via D ⁺  + OD ⁺ intermediates, from other processes leading to the same D ⁺  + D ⁺  + O final products of double ionization of water by a single photon. Moreover, we experimentally identify, separate, and follow step by step, two pathways involving the b  ¹ Σ ⁺ and a ¹ Δ electronic states of the intermediate OD ⁺ ion. Our classical trajectory calculations on the relevant potential energy surfaces reproduce well the measured data and, combined with the experiment, enable the determination of the internal energy and angular momentum distribution of the OD ⁺ intermediate.

• Research Organization: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
• Sponsoring Organization: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; USDOE Office of Science (SC), Workforce Development for Teachers and Scientists (WDTS)
• Grant/Contract Number: AC02-05CH11231; FG02-86ER13491; SC0014664
• OSTI ID: 1885176
• Journal Information: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 13; ISSN 2041-1723
• Publisher: Nature Publishing GroupCopyright Statement
• Country of Publication: United Kingdom
• Language: English