Journal ArticleDOI
Molecular dynamics with electronic transitions
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In this article, a method for carrying out molecular dynamics simulations of processes that involve electronic transitions is proposed, where the time dependent electronic Schrodinger equation is solved self-consistently with the classical mechanical equations of motion of the atoms.Abstract:
A method is proposed for carrying out molecular dynamics simulations of processes that involve electronic transitions. The time dependent electronic Schrodinger equation is solved self‐consistently with the classical mechanical equations of motion of the atoms. At each integration time step a decision is made whether to switch electronic states, according to probabilistic ‘‘fewest switches’’ algorithm. If a switch occurs, the component of velocity in the direction of the nonadiabatic coupling vector is adjusted to conserve energy. The procedure allows electronic transitions to occur anywhere among any number of coupled states, governed by the quantum mechanical probabilities. The method is tested against accurate quantal calculations for three one‐dimensional, two‐state models, two of which have been specifically designed to challenge any such mixed classical–quantal dynamical theory. Although there are some discrepancies, initial indications are encouraging. The model should be applicable to a wide variety of gas‐phase and condensed‐phase phenomena occurring even down to thermal energies.read more
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References
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Journal ArticleDOI
A new uniform semiclassical wave function for single surface and multisurface scattering
TL;DR: In this paper, a procedure for the evaluation of one-dimensional uniform semiclassical wave functions is explored, and the results are compared to the exact quantum mechanical and WKB wave functions.
Journal ArticleDOI
Intramolecular dynamics by photoelectron spectroscopy. III. Predissociation of the B̃ 2B2 state of H2O+ and D2O+ by a semiclassical approach
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Journal ArticleDOI
Electronic excitation and quenching of atoms at insulator surfaces
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