In recent years,
research focused on synthesis, characterization,
and application of metal–organic frameworks (MOFs) has attracted
increased interest, from both an experimental as well as a theoretical
perspective. Self-consistent charge density functional tight binding
(SCC DFTB) in conjunction with a suitable constrained molecular dynamics
(MD) simulation protocol provides a versatile and flexible platform
for the study of pristine MOFs as well as guest@MOF systems. Although
being a semi-empirical quantum mechanical method, SCC DFTB inherently
accounts for polarization and many-body contributions, which may become
a limiting factor in purely force field-based simulation studies.
A number of examples such as CO2, indigo, and drug molecules
embedded in various MOF hosts are discussed to highlight the capabilities
of the presented simulation approach. Furthermore, a promising extension
of the outlined simulation strategy toward the treatment of covalent
organic frameworks utilizing state-of-the-art neural network potentials
providing a description at DFT accuracy and force field cost is outlined.