Ab Initio Derived Force Fields for Zeolitic Imidazolate Frameworks: MOF-FF for ZIFs

Dürholt, J.P. and Fraux, G. and Coudert, F.-X. and Schmid, R.

Volume: 15 Pages: 2420-2432
DOI: 10.1021/acs.jctc.8b01041
Published: 2019

In this paper, we parametrized in a consistent way a new force field for a range of different zeolitic imidazolate framework systems (ZIF-8, ZIF-8(H), ZIF-8(Br), and ZIF-8(Cl)), extending the MOF-FF parametrization methodology in two aspects. First, we implemented the possibility to use periodic reference data in order to prevent the difficulty of generating representative finite clusters. Second, a new optimizer based on the covariance matrix adaptation evolutionary strategy (CMA-ES) was employed during the parametrization process. We confirmed that CMA-ES, as a state-of-the-art black box optimizer for problems on continuous variables, is more efficient and versatile for force field optimization than the previous genetic algorithm. The obtained force field was then validated with respect to some static and dynamic properties. Much effort was spent to ensure that the FF is able to describe the crucial linker swing effect in a large number of ZIF-8 derivatives. For this reason, we compared our force field to ab initio molecular dynamic simulations and found an accuracy comparable to those obtained by different exchange-correlation functionals. © 2019 American Chemical Society.

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