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Title: Photodissociation of the carbon monoxide dication in the {sup 3}Σ{sup −} manifold: Quantum control simulation towards the C{sup 2+} + O channel

The photodissociation and laser assisted dissociation of the carbon monoxide dication X{sup 3}Π CO{sup 2+} into the {sup 3}Σ{sup −} states are investigated. Ab initio electronic structure calculations of the adiabatic potential energy curves, radial nonadiabatic couplings, and dipole moments for the X {sup 3}Π state are performed for 13 excited {sup 3}Σ{sup −} states of CO{sup 2+}. The photodissociation cross section, calculated by time-dependent methods, shows that the C{sup +} + O{sup +} channels dominate the process in the studied energy range. The carbon monoxide dication CO{sup 2+} is an interesting candidate for control because it can be produced in a single, long lived, v = 0 vibrational state due to the instability of all the other excited vibrational states of the ground {sup 3}Π electronic state. In a spectral range of about 25 eV, perpendicular transition dipoles couple this {sup 3}Π state to a manifold of {sup 3}Σ{sup −} excited states leading to numerous C{sup +} + O{sup +} channels and a single C{sup 2+} + O channel. This unique channel is used as target for control calculations using local control theory. We illustrate the efficiency of this method in order to find a tailored electric field drivingmore » the photodissociation in a manifold of strongly interacting electronic states. The selected local pulses are then concatenated in a sequence inspired by the “laser distillation” strategy. Finally, the local pulse is compared with optimal control theory.« less
Authors:
 [1] ;  [2] ; ;  [1] ;  [3] ;  [4] ;  [5]
  1. Service de Chimie Quantique et Photophysique, Université Libre de Bruxelles (ULB), CP 160/09, B-1050 Brussels (Belgium)
  2. (UMR 8000), Université Paris-Sud, Orsay 91405 (France)
  3. Laboratoire Collisions Agrégats Réactivité, UMR 5589, IRSAMC, Université Toulouse III Paul Sabatier, Bât. 3R1b4, Toulouse (France)
  4. Laboratoire de Chimie Physique (UMR 8000), Univ. Paris Sud, Université Paris-Saclay, Orsay 91405 (France)
  5. (Belgium)
Publication Date:
OSTI Identifier:
22493158
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 143; Journal Issue: 16; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; 97 MATHEMATICAL METHODS AND COMPUTING; CARBON IONS; CARBON MONOXIDE; COMPARATIVE EVALUATIONS; CONTROL THEORY; CROSS SECTIONS; DIAGRAMS; DIPOLE MOMENTS; DIPOLES; DISSOCIATION; EFFICIENCY; ELECTRIC FIELDS; ELECTRONIC STRUCTURE; OPTIMAL CONTROL; OXYGEN IONS; PHOTOLYSIS; POTENTIAL ENERGY; PULSES; SIMULATION; TIME DEPENDENCE; VIBRATIONAL STATES