The QM/MM BEST method presented in the first article of this series [M. Shiga and M. Masia, J. Chem. Phys. 139, 044120 (2013)] has been applied herein to simulate the whole series of hydrated alkali ions. In this article we show how to overcome the sampling bottleneck for QM/MM simulations by using our method with multiple time scale algorithm (MTS-BEST). We extend the use of MTS-BEST to ab initio QM/MM path integral molecular dynamics simulations, thus demonstrating that one could obtain a complete quantum description of the primary subsystem based on first principles. We highlight that the MTS-BEST approach could be generally applied to hybrid multiscale simulation of diffusive systems, thus extending its relevance to a broad class of simulation techniques beyond QM/MM. We show that it is important to account for electron correlation to better reproduce the hydration structural properties such as the ion-water radial distribution functions, and the anisotropic angular distributions around the ion. (C) 2013 AIP Publishing LLC.
Boundary based on exchange symmetry theory for multilevel simulations. II. Multiple time scale approach
Masia Marco
2013
Abstract
The QM/MM BEST method presented in the first article of this series [M. Shiga and M. Masia, J. Chem. Phys. 139, 044120 (2013)] has been applied herein to simulate the whole series of hydrated alkali ions. In this article we show how to overcome the sampling bottleneck for QM/MM simulations by using our method with multiple time scale algorithm (MTS-BEST). We extend the use of MTS-BEST to ab initio QM/MM path integral molecular dynamics simulations, thus demonstrating that one could obtain a complete quantum description of the primary subsystem based on first principles. We highlight that the MTS-BEST approach could be generally applied to hybrid multiscale simulation of diffusive systems, thus extending its relevance to a broad class of simulation techniques beyond QM/MM. We show that it is important to account for electron correlation to better reproduce the hydration structural properties such as the ion-water radial distribution functions, and the anisotropic angular distributions around the ion. (C) 2013 AIP Publishing LLC.I documenti in IRIS sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.
