Daubechies Wavelets for Linear Scaling Density Functional Theory

Stephan Mohr (1) , Laura E. Ratcliff (2) , Paul Boulanger (3, 2) , Luigi Genovese (2) , Damien Caliste (2) , Thierry Deutsch (2) , Stefan Goedecker (1)

1 Unibas - Université de Bâle = University of Basel = Basel Universität
2 LSIM - Laboratory of Atomistic Simulation
3 NEEL - TMC - Théorie de la Matière Condensée

We demonstrate that Daubechies wavelets can be used to construct a minimal set of optimized localized contracted basis functions in which the Kohn-Sham orbitals can be represented with an arbitrarily high, controllable precision. Ground state energies and the forces acting on the ions can be calculated in this basis with the same accuracy as if they were calculated directly in a Daubechies wavelets basis, provided that the amplitude of these contracted basis functions is sufficiently small on the surface of the localization region, which is guaranteed by the optimization procedure described in this work. This approach reduces the computational costs of DFT calculations, and can be combined with sparse matrix algebra to obtain linear scaling with respect to the number of electrons in the system. Calculations on systems of 10,000 atoms or more thus become feasible in a systematic basis set with moderate computational resources. Further computational savings can be achieved by exploiting the similarity of the contracted basis functions for closely related environments, e.g. in geometry optimizations or combined calculations of neutral and charged systems.

Domaines: Physique [physics]

Stephan Mohr, Laura E. Ratcliff, Paul Boulanger, Luigi Genovese, Damien Caliste, et al.. Daubechies Wavelets for Linear Scaling Density Functional Theory. Journal of Chemical Physics, 2014, 140 (20), pp.204110. ⟨10.1063/1.4871876⟩. ⟨hal-01334186⟩