Fully analytic implementation of density functional theory for efficient calculations on large molecules

TL;DR

This paper introduces a fully analytic density functional theory (ADFT) model that enables efficient and accurate simulations of large molecular systems like fullerenes and nanotubes, surpassing previous computational limits.

Contribution

The authors developed a fast, variational, fully analytic DFT method that allows geometry optimization of systems with over two thousand atoms, including the largest molecule studied at this level.

Findings

Optimized geometries of large fullerenes and nanotubes containing over 2000 atoms.

Performed the largest molecule calculation (C2160) with nearly 39000 basis functions.

Studied electronic properties of inorganic cages and carbon fullerenes.

Abstract

Fullerene like cages and naonotubes of carbon and other inorganic materials are currently under intense study due to their possible technological applications. First principle simulations of these materials are computationally challenging due to large number of atoms. We have recently developed a fast, variational and fully analytic density functional theory (ADFT) based model that allows study of systems larger than those that can be studied using existing density functional models. Using polarized Gaussian basis sets (6-311G**) and ADFT, we optimize geometries of large fullerenes, fullerene-like cages and nanotubes of carbon, boron nitride, and aluminum nitride containing more than two thousand atoms. The calculation of C2160 using nearly 39000 orbital basis functions is the largest calculation on any isolated molecule reported to-date at this level of theory, and it includes full geometry optimization. The electronic structure related properties of the inorganic cages and other carbon fulerenes have been studied.