Tabletop imaging of structural evolutions in chemical reactions demonstrated for the acetylene cation

Heide Ibrahim (), Benji Wales, Samuel Beaulieu, Bruno E. Schmidt, Nicolas Thiré, Emmanuel P. Fowe, Éric Bisson, Christoph T. Hebeisen, Vincent Wanie, Mathieu Giguére, Jean-Claude Kieffer, Michael Spanner, André D. Bandrauk, Joseph Sanderson, Michael S. Schuurman and François Légaré ()
Additional contact information
Heide Ibrahim: Institut National de la Recherche Scientifique, Centre Énergie Matériaux et Télécommunications, 1650 Boulevard Lionel-Boulet
Benji Wales: University of Waterloo, 200 University Avenue West
Samuel Beaulieu: Institut National de la Recherche Scientifique, Centre Énergie Matériaux et Télécommunications, 1650 Boulevard Lionel-Boulet
Bruno E. Schmidt: Institut National de la Recherche Scientifique, Centre Énergie Matériaux et Télécommunications, 1650 Boulevard Lionel-Boulet
Nicolas Thiré: Institut National de la Recherche Scientifique, Centre Énergie Matériaux et Télécommunications, 1650 Boulevard Lionel-Boulet
Emmanuel P. Fowe: Laboratoire de Chimie Théorique, Faculté des Sciences, 2500, Boulevard de l'Université, Université de Sherbrooke
Éric Bisson: Institut National de la Recherche Scientifique, Centre Énergie Matériaux et Télécommunications, 1650 Boulevard Lionel-Boulet
Christoph T. Hebeisen: National Research Council of Canada, 100 Sussex Dr
Vincent Wanie: Institut National de la Recherche Scientifique, Centre Énergie Matériaux et Télécommunications, 1650 Boulevard Lionel-Boulet
Mathieu Giguére: Institut National de la Recherche Scientifique, Centre Énergie Matériaux et Télécommunications, 1650 Boulevard Lionel-Boulet
Jean-Claude Kieffer: Institut National de la Recherche Scientifique, Centre Énergie Matériaux et Télécommunications, 1650 Boulevard Lionel-Boulet
Michael Spanner: National Research Council of Canada, 100 Sussex Dr
André D. Bandrauk: Laboratoire de Chimie Théorique, Faculté des Sciences, 2500, Boulevard de l'Université, Université de Sherbrooke
Joseph Sanderson: University of Waterloo, 200 University Avenue West
Michael S. Schuurman: National Research Council of Canada, 100 Sussex Dr
François Légaré: Institut National de la Recherche Scientifique, Centre Énergie Matériaux et Télécommunications, 1650 Boulevard Lionel-Boulet

Nature Communications, 2014, vol. 5, issue 1, 1-8

Abstract: Abstract The introduction of femto-chemistry has made it a primary goal to follow the nuclear and electronic evolution of a molecule in time and space as it undergoes a chemical reaction. Using Coulomb Explosion Imaging, we have shot the first high-resolution molecular movie of a to and fro isomerization process in the acetylene cation. So far, this kind of phenomenon could only be observed using vacuum ultraviolet light from a free-electron laser. Here we show that 266 nm ultrashort laser pulses are capable of initiating rich dynamics through multiphoton ionization. With our generally applicable tabletop approach that can be used for other small organic molecules, we have investigated two basic chemical reactions simultaneously: proton migration and C=C bond breaking, triggered by multiphoton ionization. The experimental results are in excellent agreement with the timescales and relaxation pathways predicted by new and quantitative ab initio trajectory simulations.

Date: 2014
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DOI: 10.1038/ncomms5422

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