High-level ab initio electronic structure calculations are used to interpret the fragmentation dynamics of , following excitation with an intense ultrafast laser pulse. The potential energy surfaces of the ground and excited cationic states along the dissociative bond have been calculated using multireference second order perturbation theory methods. The calculations confirm the existence of a charge transfer resonance during the evolution of a dissociative wave packet on the ground state potential energy surface of the molecular cation and yield a detailed picture of the dissociation dynamics observed in earlier work. Comparisons of the ionic spectrum for two similar molecules support a general picture in which molecules are influenced by dynamic resonances in the cation during dissociation.
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28 March 2008
Research Article|
March 26 2008
Interpreting ultrafast molecular fragmentation dynamics with ab initio electronic structure calculations
Carlos Trallero;
Carlos Trallero
1
Staecie Institute for Molecular Sciences
, Ottawa, Ontario K1A 0R6, Canada
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Brett J. Pearson;
Brett J. Pearson
2Department of Physics and Astronomy,
Dickinson College
, Carlisle, Pennsylvania 17013, USA
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Thomas Weinacht;
Thomas Weinacht
a)
3Department of Physics and Astronomy,
Stony Brook University
, Stony Brook, New York 11794, USA
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Kandis Gilliard;
Kandis Gilliard
4Department of Chemistry,
Temple University
, Philadelphia, Pennsylvania 19122, USA
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Spiridoula Matsika
Spiridoula Matsika
b)
4Department of Chemistry,
Temple University
, Philadelphia, Pennsylvania 19122, USA
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J. Chem. Phys. 128, 124107 (2008)
Article history
Received:
December 19 2007
Accepted:
January 23 2008
Citation
Carlos Trallero, Brett J. Pearson, Thomas Weinacht, Kandis Gilliard, Spiridoula Matsika; Interpreting ultrafast molecular fragmentation dynamics with ab initio electronic structure calculations. J. Chem. Phys. 28 March 2008; 128 (12): 124107. https://doi.org/10.1063/1.2850524
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