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Adaptive molecular decomposition

Large-scale quantum chemistry for liquids
: Järvi, T.; Mayrhofer, L.; Polvi, J.; Nordlund, K.; Pastewka, L.; Moseler, M.

Postprint urn:nbn:de:0011-n-2364215 (677 KByte PDF)
MD5 Fingerprint: 3370aa56303d5df96693dda3a595849b
Erstellt am: 13.11.2013

The Journal of chemical physics 138 (2013), Nr.10, Art.104108, 10 S.
ISSN: 0021-9606
Bundesministerium für Bildung und Forschung BMBF
Zeitschriftenaufsatz, Elektronische Publikation
Fraunhofer IWM ()
benchmark testing; dissociation; electrolytes; liquid structure; molecular configurations; molecular dynamics method; quantum chemistry; SCF calculations; tight-binding calculations; water

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.