title: Accurate and efficient linear scaling DFT calculations with universal applicability.
abstract: Density functional theory calculations are computationally extremely expensive for systems containing many atoms due to their intrinsic cubic scaling. This fact has led to the development of so-called linear scaling algorithms during the last few decades. In this way it becomes possible to perform ab initio calculations for several tens of thousands of atoms within reasonable walltimes. However, even though the use of linear scaling algorithms is physically well justified, their implementation often introduces some small errors. Consequently most implementations offering such a linear complexity either yield only a limited accuracy or, if one wants to go beyond this restriction, require a tedious fine tuning of many parameters. In our linear scaling approach within the BigDFT package, we were able to overcome this restriction. Using an ansatz based on localized support functions expressed in an underlying Daubechies wavelet basis - which offers ideal properties for accurate linear scaling calculations - we obtain an amazingly high accuracy and a universal applicability while still keeping the possibility of simulating large system with linear scaling walltimes requiring only a moderate demand of computing resources. We prove the effectiveness of our method on a wide variety of systems with different boundary conditions, for single-point calculations as well as for geometry optimizations and molecular dynamics.
authors.affiliation: Université Grenoble Alpes, CEA, INAC-SP2M, F-38000 Grenoble, France. luigi.genovese@cea.fr.
authors.forename: Stephan
authors.initials: S
authors.lastname: Mohr
authors.affiliation: Université Grenoble Alpes, CEA, INAC-SP2M, F-38000 Grenoble, France. luigi.genovese@cea.fr and Argonne Leadership Computing Facility, Argonne National Laboratory, Illinois 60439, USA.
authors.forename: Laura E
authors.initials: LE
authors.lastname: Ratcliff
authors.affiliation: Université Grenoble Alpes, CEA, INAC-SP2M, F-38000 Grenoble, France. luigi.genovese@cea.fr.
authors.forename: Luigi
authors.initials: L
authors.lastname: Genovese
authors.affiliation: Université Grenoble Alpes, CEA, INAC-SP2M, F-38000 Grenoble, France. luigi.genovese@cea.fr.
authors.forename: Damien
authors.initials: D
authors.lastname: Caliste
authors.affiliation: Université Grenoble Alpes, CEA, INAC-SP2M, F-38000 Grenoble, France. luigi.genovese@cea.fr.
authors.forename: Paul
authors.initials: P
authors.lastname: Boulanger
authors.affiliation: Institut für Physik, Universität Basel, Klingelbergstr. 82, 4056 Basel, Switzerland.
authors.forename: Stefan
authors.initials: S
authors.lastname: Goedecker
authors.affiliation: Université Grenoble Alpes, CEA, INAC-SP2M, F-38000 Grenoble, France. luigi.genovese@cea.fr.
authors.forename: Thierry
authors.initials: T
authors.lastname: Deutsch