6533b7ddfe1ef96bd1273dd4
RESEARCH PRODUCT
Self-consistent field theory based molecular dynamics with linear system-size scaling
Dorothee RichtersThomas D. Kühnesubject
PhysicsChemical Physics (physics.chem-ph)Condensed Matter - Materials ScienceField (physics)Linear systemBorn–Oppenheimer approximationGeneral Physics and AstronomyMaterials Science (cond-mat.mtrl-sci)FOS: Physical sciencesComputational Physics (physics.comp-ph)Langevin equationMolecular dynamicssymbols.namesakePhysics - Chemical PhysicssymbolsLinear scaleEnergy driftStatistical physicsPhysical and Theoretical ChemistryPhysics - Computational PhysicsScalingdescription
We present an improved field-theoretic approach to the grand-canonical potential suitable for linear scaling molecular dynamics simulations using forces from self-consistent electronic structure calculations. It is based on an exact decomposition of the grand canonical potential for independent fermions and does neither rely on the ability to localize the orbitals nor that the Hamilton operator is well-conditioned. Hence, this scheme enables highly accurate all-electron linear scaling calculations even for metallic systems. The inherent energy drift of Born-Oppenheimer molecular dynamics simulations, arising from an incomplete convergence of the self-consistent field cycle, is circumvented by means of a properly modified Langevin equation. The predictive power of the present linear scaling \textit{ab-initio} molecular dynamics approach is illustrated using the example of liquid methane under extreme conditions.
| year | journal | country | edition | language |
|---|---|---|---|---|
| 2012-06-23 |