Universal QM/MM Approaches for General Nanoscale Applications

Abstract

Hybrid quantum mechanics/molecular mechanics (QM/MM) hybrid models allow one to address chemical phenomena in complex molecular environments. However, they are tedious to construct and they usually require significant manual preprocessing and expertise. As a result, these models may not be easily transferable to new application areas and the many parameters are not easy to adjust to reference data that are typically scarce. Therefore, it has been difficult to devise automated procedures of controllable accuracy, which makes such type of modelling far from being standardized or of black-box type. Although diverse best-practice protocols have been set up for the construction of individual components of a QM/MM model (e.g., the MM potential, the type of embedding, the choice of the QM region), no automated procedures are available for all steps of the QM/MM model construction. Here, we review the state of the art of QM/MM modeling with a focus on automation. We elaborate on the MM model parametrization, on atom-economical physically-motivated QM region selection, and on embedding schemes that incorporate mutual polarization as critical components of the QM/MM model. In view of the broad scope of the field, we mostly restrict the discussion to methodologies that build de novo models based on first-principles data, on uncertainty quantification, and on error mitigation with a high potential for automation. Ultimately, it is desirable to be able to set up reliable QM/MM models in a fast and efficient automated way without being constrained by some specific chemical or technical limitations.

Development of a Transferable Force Field between Metal–Organic Framework and Its Polymorph

“…This methodology is economical and promising, yet problems of automation still exist. 26 Although numerous state-of-the-art technologies introduced here are actively utilized for economic force field developments, problems of specificity and applicability remain challenges. In other words, an extension of these force fields is required as they often fail to accurately describe diverse and uncommon building blocks or conditions.…”