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

Travis Severt, Zachary L. Streeter, Wael Iskandar, Kirk A. Larsen, Averell Gatton, Daniel Trabert, Bethany Jochim, Brandon Griffin, Elio G. Champenois, Matthew M. Brister, Dylan Reedy, Demitri Call, Richard Strom, Allen L. Landers, Reinhard Dörner, Joshua B. Williams, Daniel S. Slaughter, Robert R. Lucchese, Thorsten Weber (), C. William McCurdy () and Itzik Ben-Itzhak ()
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Travis Severt: Kansas State University
Zachary L. Streeter: Lawrence Berkeley National Laboratory
Wael Iskandar: Lawrence Berkeley National Laboratory
Kirk A. Larsen: Lawrence Berkeley National Laboratory
Averell Gatton: Lawrence Berkeley National Laboratory
Daniel Trabert: Goethe-Universität
Bethany Jochim: Kansas State University
Brandon Griffin: Lawrence Berkeley National Laboratory
Elio G. Champenois: Lawrence Berkeley National Laboratory
Matthew M. Brister: Lawrence Berkeley National Laboratory
Dylan Reedy: University of Nevada Reno
Demitri Call: University of Nevada Reno
Richard Strom: Lawrence Berkeley National Laboratory
Allen L. Landers: Auburn University
Reinhard Dörner: Goethe-Universität
Joshua B. Williams: University of Nevada Reno
Daniel S. Slaughter: Lawrence Berkeley National Laboratory
Robert R. Lucchese: Lawrence Berkeley National Laboratory
Thorsten Weber: Lawrence Berkeley National Laboratory
C. William McCurdy: Lawrence Berkeley National Laboratory
Itzik Ben-Itzhak: Kansas State University

Nature Communications, 2022, vol. 13, issue 1, 1-9

Abstract: 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 1Σ+ and a 1Δ 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.

Date: 2022
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DOI: 10.1038/s41467-022-32836-6

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