18 research outputs found
Ab initio molecular dynamics simulations of Aluminum solvation
The solvation of Al and its hydrolyzed species in water clusters has been
studied by means of ab initio molecular dynamics simulations. The hexa-hydrate
aluminum ion formed a stable complex in the finite temperature cluster
simulation of one aluminum ion and 16 waters. The average dipole moment of
strongly polarized hydrated water molecules in the first solvation shell of the
hexa-hydrate aluminum ion was found to be 5.02 Debye. The deprotonated
hexa-hydrate complex evolves into a tetra-coordinated aluminate ion with two
water molecules in the second solvation shell forming hydrogen bonds to the
hydroxyl groups in agreement with the observed coordination.Comment: 12 pages in Elsevier LaTeX, 5 figures in Postscript, 2 last figures
are in color, submitted to Chemical Physics Letter
Ab initio many-body calculations on infinite carbon and boron-nitrogen chains
In this paper we report first-principles calculations on the ground-state
electronic structure of two infinite one-dimensional systems: (a) a chain of
carbon atoms and (b) a chain of alternating boron and nitrogen atoms. Meanfield
results were obtained using the restricted Hartree-Fock approach, while the
many-body effects were taken into account by second-order M{\o}ller-Plesset
perturbation theory and the coupled-cluster approach. The calculations were
performed using 6-31 basis sets, including the d-type polarization
functions. Both at the Hartree-Fock (HF) and the correlated levels we find that
the infinite carbon chain exhibits bond alternation with alternating single and
triple bonds, while the boron-nitrogen chain exhibits equidistant bonds. In
addition, we also performed density-functional-theory-based local density
approximation (LDA) calculations on the infinite carbon chain using the same
basis set. Our LDA results, in contradiction to our HF and correlated results,
predict a very small bond alternation. Based upon our LDA results for the
carbon chain, which are in agreement with an earlier LDA calculation
calculation [ E.J. Bylaska, J.H. Weare, and R. Kawai, Phys. Rev. B 58, R7488
(1998).], we conclude that the LDA significantly underestimates Peierls
distortion. This emphasizes that the inclusion of many-particle effects is very
important for the correct description of Peierls distortion in one-dimensional
systems.Comment: 3 figures (included). To appear in Phys. Rev.
Ion association in AlCl3 aqueous solutions from Constrained First Principles Molecular Dynamics
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Ab initio molecular dynamics of aqueous 2+ and 3+ cations: a model of the 2nd hydration shell
info:eu-repo/semantics/nonPublishe
Ab initio molecular dynamics simulations of the hydration shells of highly charged metal ions in aqueous solutions
info:eu-repo/semantics/nonPublishe
1st principle simulation of H-bonding structure, ion association, and proton and ligand transfer reactions in metal ion hydration shells under ambient and extreme conditions
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Predicting the chemical and physical properties of geothermal fluids: Model development and molecular level theoretical understanding
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Predicting the chemical and physical properties of geothermal fluids :Model development and molecular level theoretical understanding
info:eu-repo/semantics/nonPublishe
First principle dynamical simulation of hydrogen bond structure, dynamics and simple reactions in the hydration shells of highly charged metal ions
info:eu-repo/semantics/publishe