Journal
JOURNAL OF CHEMICAL PHYSICS
Volume 137, Issue 6, Pages -Publisher
AMER INST PHYSICS
DOI: 10.1063/1.4742816
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Funding
- National Science Foundation [CHE-0748448]
- Ohio Supercomputer Center [PAS-0291]
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [0748448] Funding Source: National Science Foundation
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Fragment-based quantum chemistry methods are a promising route towards massively parallel electronic structure calculations in large systems. Unfortunately, the literature on this topic consists of a bewildering array of different methods, with no clear guiding principles to choose amongst them. Here, we introduce a conceptual framework that unifies many of these ostensibly disparate approaches. The common framework is based upon an approximate supersystem energy formula for a collection of intersecting (i.e., overlapping) fragments. This formula generalizes the traditional many-body expansion to cases where the bodies (fragments) share some nuclei in common, and reduces to the traditional many-body expansion for non-overlapping fragments. We illustrate how numerous fragment-based methods fit within this framework. Preliminary applications to molecular and ionic clusters suggest that two-body methods in which dimers are constructed from intersecting fragments may be a route to achieve very high accuracy in fragment-based calculations. (C) 2012 American Institute of Physics. [http://dx.doi.org/10.1063/1.4742816]
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