title: Full-dimensional control of the radiationless decay in pyrazine using the dynamic Stark effect.
abstract: We present a full quantum-mechanical study of the laser control of the radiationless decay between the B3u(nπ(*)) and B2u(ππ(*)) states of pyrazine using the dynamic Stark effect. In contrast to our previous study [Sala et al., J. Chem. Phys. 140, 194309 (2014)], where a four-dimensional model was used, all the 24 degrees of freedom are now included in order to test the robustness of the strategy of control. Using a vibronic coupling Hamiltonian model in a diabatic representation, the multi-layer version of the multi-configuration time-dependent Hartree method is exploited to propagate the corresponding wave packets. We still observe a trapping of the wavepacket on the B2u(ππ(*)) potential energy surface due to the Stark effect for a longer time than the "non-resonant field-free" B2u(ππ(*)) lifetime.
authors.affiliation: CTMM, Institut Charles Gerhardt Montpellier (UMR5253), CC 15001, Université Montpellier 2, F-34095 Montpellier, Cedex 05, France.
authors.forename: Mohamad
authors.initials: M
authors.lastname: Saab
authors.affiliation: Laboratoire Interdisciplinaire Carnot de Bourgogne (UMR 6303) CNRS, Université de Bourgogne, BP 47870, F-21078 Dijon, France.
authors.forename: Matthieu
authors.initials: M
authors.lastname: Sala
authors.affiliation: CTMM, Institut Charles Gerhardt Montpellier (UMR5253), CC 15001, Université Montpellier 2, F-34095 Montpellier, Cedex 05, France.
authors.forename: Benjamin
authors.initials: B
authors.lastname: Lasorne
authors.affiliation: CTMM, Institut Charles Gerhardt Montpellier (UMR5253), CC 15001, Université Montpellier 2, F-34095 Montpellier, Cedex 05, France.
authors.forename: Fabien
authors.initials: F
authors.lastname: Gatti
authors.affiliation: Laboratoire Interdisciplinaire Carnot de Bourgogne (UMR 6303) CNRS, Université de Bourgogne, BP 47870, F-21078 Dijon, France.
authors.forename: Stéphane
authors.initials: S
authors.lastname: Guérin