Calibration of forcefields for molecular simulation: Sequential design of computer experiments for building cost-efficient kriging metamodels
Article first published online: 25 OCT 2013
Copyright © 2013 Wiley Periodicals, Inc.
Journal of Computational Chemistry
Volume 35, Issue 2, pages 130–149, 15 January 2014
How to Cite
How to cite this article: J. Comput. Chem. 2014, 35, 130-149. DOI: 10.1002/jcc.23475., , .
- Issue published online: 8 DEC 2013
- Article first published online: 25 OCT 2013
- Manuscript Accepted: 6 OCT 2013
- Manuscript Revised: 23 AUG 2013
- Manuscript Received: 8 APR 2013
- molecular simulation;
- forcefield calibration;
- efficient global optimization;
- uncertainty quantification
We present a global strategy for molecular simulation forcefield optimization, using recent advances in Efficient Global Optimization algorithms. During the course of the optimization process, probabilistic kriging metamodels are used, that predict molecular simulation results for a given set of forcefield parameter values. This enables a thorough investigation of parameter space, and a global search for the minimum of a score function by properly integrating relevant uncertainty sources. Additional information about the forcefield parameters are obtained that are inaccessible with standard optimization strategies. In particular, uncertainty on the optimal forcefield parameters can be estimated, and transferred to simulation predictions. This global optimization strategy is benchmarked on the TIP4P water model. © 2013 Wiley Periodicals, Inc.