Application of a coupled-surface time-dependent Hartree grid method to excited state optical spectroscopy

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Abstract
The dynamics of multidimensional wave packet motion on nonadiabatically coupled electronic potential surfaces is explored by numerically exact time¿dependent quantum mechanics and by the time¿dependent Hartree grid (TDHG) approximation. Excellent agreement is found between the TDHG and the exact evolution of the wave packet; in particular, the approximation yields accurate total cross sections for electronic absorption, excitation profiles for resonance Raman scattering, and partial cross sections for photofragmentation in a two degree of freedom model of direct dissociation (which is qualitatively related to experimentally observed processes in methyl halides and ICN).@ American Institute of PhysicsThis work was supported by a grant from the National Science Foundation, the Petroleum Research Fund, the Alfred P. Sloan Foundation, and the Camille and Henry Dreyfus Foundation. J. C.-M. gratefully acknowledges a grant from the Ministerio de Educacion y Ciencia of SpainPeer Reviewe