Coulomb explosion imaging of small polyatomic molecules with ultrashort x-ray pulses

Abstract

Ultrashort x-ray pulses from free-electron lasers can efficiently charge up and trigger the full fragmentation of molecules. By coincident detection of up to five ions resulting from rapid Coulomb explosion of highly charged iodomethane, we show that the full three-dimensional equilibrium geometry of this prototypical polyatomic system can be determined from the measured ion momenta with the help of a charge buildup model. Supported by simulations of how the ion momenta would reflect specific changes in molecular bond lengths and angles, we demonstrate that Coulomb-explosion imaging with ultrashort x-ray pulses is a promising technique for recording movies of multidimensional nuclear wave packets, including hydrogen motions.Received 18 January 2021Revised 22 September 2021Accepted 23 September 2021DOI:https://doi.org/10.1103/PhysRevResearch.4.013029Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.Published by the American Physical SocietyPhysics Subject Headings (PhySH)Research AreasAtomic & molecular processes in external fieldsAtomic & molecular structureLight-matter interactionSingle- and few-photon ionization & excitationUltrafast phenomenaX-ray beams & opticsAtomic, Molecular & Optical