Communication: Improved ab initio molecular dynamics by minimally biasing with experimental data.
Accounting for electrons and nuclei simultaneously is a powerful capability of ab initio molecular dynamics (AIMD). However, AIMD is often unable to accurately reproduce properties of systems such as water due to inaccuracies in the underlying electronic density functionals. This shortcoming is often addressed by added empirical corrections and/or increasing the simulation temperature. We present here a maximum-entropy approach to directly incorporate limited experimental data via a minimal bias. Biased AIMD simulations of water and an excess proton in water are shown to give significantly improved properties both for observables which were biased to match experimental data and for unbiased observables. This approach also yields new physical insight into inaccuracies in the underlying density functional theory as utilized in the unbiased AIMD.
Department of Chemistry, James Franck Institute, and Institute for Biophysical Dynamics, The University of Chicago, 5735 S Ellis Ave., Chicago, Illinois 60637, USA.
Andrew D
AD
White
Leadership Computing Facility, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, Illinois 60439, USA.
Chris
0000000184320658
C
Knight
Department of Chemistry, James Franck Institute, and Institute for Biophysical Dynamics, The University of Chicago, 5735 S Ellis Ave., Chicago, Illinois 60637, USA.
Glen M
0000000256370698
GM
Hocky
Department of Chemistry, James Franck Institute, and Institute for Biophysical Dynamics, The University of Chicago, 5735 S Ellis Ave., Chicago, Illinois 60637, USA.
Gregory A
0000000232676748
GA
Voth