215832
20190317000404.0
1089-7690
10.1063/1.4941091
doi
000369893900013
ISI
ARTICLE
Accurate molecular dynamics and nuclear quantum effects at low cost by multiple steps in real and imaginary time: Using density functional theory to accelerate wavefunction methods
Melville
2016
American Institute of Physics
2016
6
Journal Articles
The development and implementation of increasingly accurate methods for electronic structure calculations mean that, for many atomistic simulation problems, treating light nuclei as classical particles is now one of the most serious approximations. Even though recent developments have significantly reduced the overhead for modeling the quantum nature of the nuclei, the cost is still prohibitive when combined with advanced electronic structure methods. Here we present how multiple time step integrators can be combined with ring-polymer contraction techniques (effectively, multiple time stepping in imaginary time) to reduce virtually to zero the overhead of modelling nuclear quantum effects, while describing inter-atomic forces at high levels of electronic structure theory. This is demonstrated for a combination of MP2 and semi-local DFT applied to the Zundel cation. The approach can be seamlessly combined with other methods to reduce the computational cost of path integral calculations, such as high-order factorizations of the Boltzmann operator or generalized Langevin equation thermostats. (C) 2016 AIP Publishing LLC.
Kapil, V.
263953
249520
Vandevondele, J.
Ceriotti, M.
235586
247464
054111
5
The Journal of Chemical Physics
144
Preprint
982773
Preprint
http://infoscience.epfl.ch/record/215832/files/1512.00176v1.pdf
COSMO
252486
U12743
oai:infoscience.tind.io:215832
article
STI
GLOBAL_SET
235586
EPFL-ARTICLE-215832
EPFL
PUBLISHED
NON-REVIEWED
ARTICLE