Full-dimensional control of the radiationless decay in pyrazine using the dynamic Stark effect

Journal Article · Tue Oct 07 04:00:00 EDT 2014 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4896938· OSTI ID:22436541

Saab, Mohamad; Lasorne, Benjamin; Gatti, Fabien ^[1]; Sala, Matthieu; Guérin, Stéphane ^[2]

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1. CTMM, Institut Charles Gerhardt Montpellier (UMR5253), CC 15001, Université Montpellier 2, F-34095 Montpellier, Cedex 05 (France)
2. Laboratoire Interdisciplinaire Carnot de Bourgogne (UMR 6303) CNRS, Université de Bourgogne, BP 47870, F-21078 Dijon (France)

We present a full quantum-mechanical study of the laser control of the radiationless decay between the B{sub 3u}(nπ{sup *}) and B{sub 2u}(ππ{sup *}) 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 B{sub 2u}(ππ{sup *}) potential energy surface due to the Stark effect for a longer time than the “non-resonant field-free” B{sub 2u}(ππ{sup *}) lifetime.

• OSTI ID: 22436541
• Journal Information: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 13 Vol. 141; ISSN JCPSA6; ISSN 0021-9606
• Country of Publication: United States
• Language: English

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
71 CLASSICAL AND QUANTUM MECHANICS
GENERAL PHYSICS
CONTROL
COUPLING
DEGREES OF FREEDOM
HAMILTONIANS
POTENTIAL ENERGY
RADIATIONLESS DECAY
STARK EFFECT
SURFACES
TIME DEPENDENCE
WAVE PACKETS