title: Adaptive molecular decomposition: 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.
authors.affiliation: Fraunhofer Institute for Mechanics of Materials IWM, Wöhlerstrasse 11, D-79108 Freiburg, Germany.
authors.forename: Tommi T
authors.initials: TT
authors.lastname: Järvi
authors.forename: Leonhard
authors.initials: L
authors.lastname: Mayrhofer
authors.forename: Jussi
authors.initials: J
authors.lastname: Polvi
authors.forename: Kai
authors.initials: K
authors.lastname: Nordlund
authors.forename: Lars
authors.initials: L
authors.lastname: Pastewka
authors.forename: Michael
authors.initials: M
authors.lastname: Moseler