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Filming enhanced ionization in an ultrafast triatomic slingshot

Andrew J. Howard, Mathew Britton, Zachary Streeter, Chuan Cheng, Ruaridh Forbes, Joshua L. Reynolds, Felix Allum, Gregory A. McCracken, Ian Gabalski, Robert R. Lucchese, C. William McCurdy, Thomas Weinacht, P. H. Bucksbaum

2023Communications Chemistry23 citationsDOIOpen Access PDF

Abstract

Filming atomic motion within molecules is an active pursuit of molecular physics and quantum chemistry. A promising method is laser-induced Coulomb Explosion Imaging (CEI) where a laser pulse rapidly ionizes many electrons from a molecule, causing the remaining ions to undergo Coulomb repulsion. The ion momenta are used to reconstruct the molecular geometry which is tracked over time (i.e., filmed) by ionizing at an adjustable delay with respect to the start of interatomic motion. Results are distorted, however, by ultrafast motion during the ionizing pulse. We studied this effect in water and filmed the rapid "slingshot" motion that enhances ionization and distorts CEI results. Our investigation uncovered both the geometry and mechanism of the enhancement which may inform CEI experiments in many other polyatomic molecules.

Topics & Concepts

Triatomic moleculeIonizationUltrashort pulseAtomic physicsChemistryPhysicsOpticsLaserIonQuantum mechanicsMoleculeLaser-Matter Interactions and ApplicationsIon-surface interactions and analysisSpectroscopy and Quantum Chemical Studies
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