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Expanding the Scope of Density Derived Electrostatic and Chemical Charge Partitioning to Thousands of Atoms

Lookup NU author(s): Dr Daniel Cole

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Abstract

The density derived electrostatic and chemical (DDEC/c3) method is implemented into the onetep program to compute net atomic charges (NACs), as well as higher-order atomic multipole moments, of molecules, dense solids, nanoclusters, liquids, and biomolecules using linear-scaling density functional theory (DFT) in a distributed memory parallel computing environment. For a >1000 atom model of the oxygenated myoglobin protein, the DDEC/c3 net charge of the adsorbed oxygen molecule is approximately −1e (in agreement with the Weiss model) using a dynamical mean field theory treatment of the iron atom, but much smaller in magnitude when using the generalized gradient approximation. For GaAs semiconducting nanorods, the system dipole moment using the DDEC/c3 NACs is about 5% higher in magnitude than the dipole computed directly from the quantum mechanical electron density distribution, and the DDEC/c3 NACs reproduce the electrostatic potential to within approximately 0.1 V on the nanorod’s solvent-accessible surface. As examples of conducting materials, we study (i) a 55-atom Pt cluster with an adsorbed CO molecule and (ii) the dense solids Mo2C and Pd3V. Our results for solid Mo2C and Pd3V confirm the necessity of a constraint enforcing exponentially decaying electron density in the tails of buried atoms.


Publication metadata

Author(s): Lee LP, Gabaldon Limas N, Cole DJ, Payne MC, Skylaris C-K, Manz TA

Publication type: Article

Publication status: Published

Journal: Journal of Chemical Theory and Computation

Year: 2014

Volume: 10

Issue: 12

Pages: 5377-5390

Online publication date: 03/11/2014

Acceptance date: 03/11/2014

ISSN (print): 15499626

ISSN (electronic): 15499618

Publisher: American Chemical Society

URL: http://dx.doi.org/10.1021/ct500766v

DOI: 10.1021/ct500766v


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