Ab initio quantum mechanical charge field (QMCF) molecular dynamics: a QM/MM – MD procedure for accurate simulations of ions and complexes |
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Authors: | Bernd M Rode Thomas S Hofer Bernhard R Randolf Christian F Schwenk Demetrios Xenides Viwat Vchirawongkwin |
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Institution: | (1) Theoretical Chemistry Division, Institute of General, Inorganic and Theoretical Chemistry, University of Innsbruck, Innrain 52a, A-6020 Innsbruck, Austria |
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Abstract: | A new formalism for quantum mechanical / molecular mechanical (QM/MM) dynamics of chemical species in solution has been developed,
which does not require the construction of any other potential functions except those for solvent–solvent interactions, maintains
all the advantages of large simulation boxes and ensures the accuracy of ab initio quantum mechanics for all forces acting
in the chemically most relevant region. Interactions between solute and more distant solvent molecules are incorporated by
a dynamically adjusted force field corresponding to the actual molecular configuration of the simulated system and charges
derived from the electron distribution in the solvate. The new formalism has been tested with some examples of hydrated ions,
for which accurate conventional ab initio QM/MM simulations have been previously performed, and the comparison shows equivalence
and in some aspects superiority of the new method. As this simulation procedure does not require any tedious construction
of two-and three-body interaction potentials inherent to conventional QM/MM approaches, it opens the straightforward access
to ab initio molecular dynamics simulations of any kind of solutes, such as metal complexes and other composite species in
solution. |
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