title: Efficient Linear-Scaling Density Functional Theory for Molecular Systems.
abstract: Despite recent progress in linear scaling (LS) density function theory (DFT), the computational cost of the existing LS methods remains too high for a widespread adoption at present. In this work, we exploit nonorthogonal localized molecular orbitals to develop a series of LS methods for molecular systems with a low computational overhead. High efficiency of the proposed methods is achieved with a new robust two-stage variational procedure or by replacing the optimization altogether with an accurate nonself-consistent approach. We demonstrate that, even for challenging condensed-phase systems, the implemented LS methods are capable of extending the range of accurate DFT simulations to molecular systems that are an order of magnitude larger than those previously treated.
authors.affiliation: Physical Chemistry Institute, University of Zürich , Winterthurerstrasse 180, 8057 Zürich, Switzerland.|Institute of Physical Chemistry, Johannes Gutenberg University of Mainz , Staudingerweg 7, 55128 Mainz, Germany.
authors.forename: Rustam Z
authors.initials: RZ
authors.lastname: Khaliullin
authors.affiliation: Department of Materials, Swiss Federal Institute of Technology , Wolfgang-Pauli-Strasse 27, 8093 Zürich, Switzerland.
authors.forename: Joost
authors.initials: J
authors.lastname: VandeVondele
authors.affiliation: Physical Chemistry Institute, University of Zürich , Winterthurerstrasse 180, 8057 Zürich, Switzerland.
authors.forename: Jürg
authors.initials: J
authors.lastname: Hutter