title: Tabletop imaging of structural evolutions in chemical reactions demonstrated for the acetylene cation.
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.
authors.affiliation: Institut National de la Recherche Scientifique, Centre Énergie Matériaux et Télécommunications, 1650 Boulevard Lionel-Boulet, Varennes, Quebec, Canada J3X 1S2.
authors.forename: Heide
authors.initials: H
authors.lastname: Ibrahim
authors.affiliation: Department of Physics and Astronomy, University of Waterloo, 200 University Avenue West, Waterloo, Ontario, Canada N2L 3G1.
authors.forename: Benji
authors.initials: B
authors.lastname: Wales
authors.affiliation: Institut National de la Recherche Scientifique, Centre Énergie Matériaux et Télécommunications, 1650 Boulevard Lionel-Boulet, Varennes, Quebec, Canada J3X 1S2.
authors.forename: Samuel
authors.initials: S
authors.lastname: Beaulieu
authors.affiliation: Institut National de la Recherche Scientifique, Centre Énergie Matériaux et Télécommunications, 1650 Boulevard Lionel-Boulet, Varennes, Quebec, Canada J3X 1S2.
authors.forename: Bruno E
authors.initials: BE
authors.lastname: Schmidt
authors.affiliation: Institut National de la Recherche Scientifique, Centre Énergie Matériaux et Télécommunications, 1650 Boulevard Lionel-Boulet, Varennes, Quebec, Canada J3X 1S2.
authors.forename: Nicolas
authors.initials: N
authors.lastname: Thiré
authors.affiliation: Laboratoire de Chimie Théorique, Faculté des Sciences, 2500, Boulevard de l'Université, Université de Sherbrooke, Quebec, Canada J1K 2R1.
authors.forename: Emmanuel P
authors.initials: EP
authors.lastname: Fowe
authors.affiliation: Institut National de la Recherche Scientifique, Centre Énergie Matériaux et Télécommunications, 1650 Boulevard Lionel-Boulet, Varennes, Quebec, Canada J3X 1S2.
authors.forename: Éric
authors.initials: É
authors.lastname: Bisson
authors.affiliation: 1] National Research Council of Canada, 100 Sussex Dr, Ottawa, Ontario, Canada K1A 0R6 [2] Department of Physics, University of Ottawa, 150 Louis Pasteur, Ottawa Ontario, Canada K1N 6N5.
authors.forename: Christoph T
authors.initials: CT
authors.lastname: Hebeisen
authors.affiliation: Institut National de la Recherche Scientifique, Centre Énergie Matériaux et Télécommunications, 1650 Boulevard Lionel-Boulet, Varennes, Quebec, Canada J3X 1S2.
authors.forename: Vincent
authors.initials: V
authors.lastname: Wanie
authors.affiliation: Institut National de la Recherche Scientifique, Centre Énergie Matériaux et Télécommunications, 1650 Boulevard Lionel-Boulet, Varennes, Quebec, Canada J3X 1S2.
authors.forename: Mathieu
authors.initials: M
authors.lastname: Giguére
authors.affiliation: Institut National de la Recherche Scientifique, Centre Énergie Matériaux et Télécommunications, 1650 Boulevard Lionel-Boulet, Varennes, Quebec, Canada J3X 1S2.
authors.forename: Jean-Claude
authors.initials: JC
authors.lastname: Kieffer
authors.affiliation: National Research Council of Canada, 100 Sussex Dr, Ottawa, Ontario, Canada K1A 0R6.
authors.forename: Michael
authors.initials: M
authors.lastname: Spanner
authors.affiliation: Laboratoire de Chimie Théorique, Faculté des Sciences, 2500, Boulevard de l'Université, Université de Sherbrooke, Quebec, Canada J1K 2R1.
authors.forename: André D
authors.initials: AD
authors.lastname: Bandrauk
authors.affiliation: Department of Physics and Astronomy, University of Waterloo, 200 University Avenue West, Waterloo, Ontario, Canada N2L 3G1.
authors.forename: Joseph
authors.initials: J
authors.lastname: Sanderson
authors.affiliation: National Research Council of Canada, 100 Sussex Dr, Ottawa, Ontario, Canada K1A 0R6.
authors.forename: Michael S
authors.initials: MS
authors.lastname: Schuurman
authors.affiliation: Institut National de la Recherche Scientifique, Centre Énergie Matériaux et Télécommunications, 1650 Boulevard Lionel-Boulet, Varennes, Quebec, Canada J3X 1S2.
authors.forename: François
authors.initials: F
authors.lastname: Légaré