ct9b01152_si_001.zip (1.86 MB)
Complexity Reduction in Density Functional Theory Calculations of Large Systems: System Partitioning and Fragment Embedding
dataset
posted on 2020-04-09, 14:42 authored by William Dawson, Stephan Mohr, Laura E. Ratcliff, Takahito Nakajima, Luigi GenoveseWith the development
of low order scaling methods for performing
Kohn–Sham density functional theory, it is now possible to
perform fully quantum mechanical calculations of systems containing
tens of thousands of atoms. However, with an increase in the size
of the system treated comes an increase in complexity, making it challenging
to analyze such large systems and determine the cause of emergent
properties. To address this issue, in this paper, we present a systematic
complexity reduction methodology which can break down large systems
into their constituent fragments and quantify interfragment interactions.
The methodology proposed here requires no a priori information or
user interaction, allowing a single workflow to be automatically applied
to any system of interest. We apply this approach to a variety of
different systems and show how it allows for the derivation of new
system descriptors, the design of QM/MM partitioning schemes, and
the novel application of graph metrics to molecules and materials.