A general method for implementing vibrationally adiabatic mixed quantum-classical simulations

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Issue Date
2003-01-06Author
Thompson, Ward H.
Publisher
American Institute of Physics
Type
Article
Article Version
Scholarly/refereed, publisher version
Metadata
Show full item recordAbstract
An approach for carrying out vibrationally adiabatic mixed quantum-classical molecular dynamics simulations is presented. An appropriate integration scheme is described for the vibrationally adiabatic equations of motion of a diatomic solute in a monatomic solvent and an approach for calculating the adiabatic energy levels is presented. Specifically, an iterative Lanczos algorithm with full reorthogonalization is used to solve for the lowest few vibrational eigenvalues and eigenfunctions. The eigenfunctions at one time step in a mixed quantum-classical trajectory are used to initiate the Lanczos calculation at the next time step. The basis set size is reduced by using a potential-optimized discrete variable representation. As a demonstration the problem of a homonuclear diatomic molecule in a rare gas fluid (N2 in Ar) has been treated. The approach is shown to be efficient and accurate. An important advantage of this approach is that it can be straightforwardly applied to polyatomic solutes that have multiple vibrational degrees-of-freedom that must be quantized.
Description
This is the publisher's version, also available electronically from http://scitation.aip.org/content/aip/journal/jcp/118/3/10.1063/1.1528891.
ISSN
0021-9606Collections
Citation
Thompson, Ward H. (2003). "A general method for implementing vibrationally adiabatic mixed quantum-classical simulations." The Journal of Chemical Physics, 118(3):1059-1067. http://dx.doi.org/10.1063/1.1528891
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