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2013
Journal Article
Titel

Adaptive molecular decomposition

Titel Supplements
Large-scale quantum chemistry for liquids
Abstract
We present a linear-scaling method based on self-consistent charge non-orthogonal tight-binding. Linear scaling is achieved using a many-body expansion, which is adjusted dynamically to the instantaneous molecular configuration of a liquid. The method is capable of simulating liquids over large length and time scales, and also handles reactions correctly. Benchmarking on typical carbonate electrolytes used in Li-ion batteries displays excellent agreement with results from full tight-binding calculations. The decomposition slightly breaks the Hellmann-Feynman theorem, which is demonstrated by application to water. However, an additional correction also enables dynamical simulation in this case.
Author(s)
Järvi, T.
Mayrhofer, L.
Polvi, J.
Nordlund, K.
Pastewka, L.
Moseler, M.
Zeitschrift
The Journal of chemical physics
Funder
Bundesministerium für Bildung und Forschung BMBF (Deutschland)
DOI
10.1063/1.4793708
File(s)
001.pdf (677.8 KB)
Language
English
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Fraunhofer-Institut für Werkstoffmechanik IWM
Tags
  • benchmark testing

  • dissociation

  • electrolytes

  • liquid structure

  • molecular configurations

  • molecular dynamics method

  • quantum chemistry

  • SCF calculations

  • tight-binding calculations

  • water

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