Flexible Force Field Parameterization through Fitting on the Ab Initio-Derived Elastic Tensor

Constructing functional forms and their corresponding force field parameters for the metal–linker interface of metal–organic frameworks is challenging. We propose fitting these parameters on the elastic tensor, computed from ab initio density functional theory calculations. The advantage of this top...

Full description

Saved in:
Bibliographic Details
Published inJournal of chemical theory and computation Vol. 13; no. 8; pp. 3722 - 3730
Main Authors Heinen, Jurn, Burtch, Nicholas C, Walton, Krista S, Dubbeldam, David
Format Journal Article
LanguageEnglish
Published United States American Chemical Society 08.08.2017
Subjects
Density functional theory
Mechanical properties
Molecular chains
Parameterization
Parameters
Periodic structures
Thermal expansion
Online AccessGet full text

Cover

More Information
Summary:Constructing functional forms and their corresponding force field parameters for the metal–linker interface of metal–organic frameworks is challenging. We propose fitting these parameters on the elastic tensor, computed from ab initio density functional theory calculations. The advantage of this top-down approach is that it becomes evident if functional forms are missing when components of the elastic tensor are off. As a proof-of-concept, a new flexible force field for MIL-47­(V) is derived. Negative thermal expansion is observed and framework flexibility has a negligible effect on adsorption and transport properties for small guest molecules. We believe that this force field parametrization approach can serve as a useful tool for developing accurate flexible force field models that capture the correct mechanical behavior of the full periodic structure.
Bibliography:ObjectType-Article-1
SourceType-Scholarly Journals-1
ObjectType-Feature-2
content type line 23
ISSN:1549-9618
1549-9626
DOI:10.1021/acs.jctc.7b00310