Probing the range of applicability of structure‐ and energy‐adjusted QM/MM link bonds III: QM/MM MD simulations of solid‐state systems at the example of layered carbon structures

Abstract

AbstractThe previously introduced workflow to achieve an energetically and structurally optimized description of frontier bonds in quantum mechanical/molecular mechanics (QM/MM)‐type applications was extended into the regime of computational material sciences at the example of a layered carbon model systems. Optimized QM/MM link bond parameters at HSEsol/6‐311G(d,p) and self‐consistent density functional tight binding (SCC‐DFTB) were derived for graphitic systems, enabling detailed investigation of specific structure motifs occurring in graphene‐derived structures quantum‐chemical calculations. Exemplary molecular dynamics (MD) simulations in the isochoric‐isothermic (NVT) ensemble were carried out to study the intercalation of lithium and the properties of the Stone–Thrower–Wales defect. The diffusivity of lithium as well as hydrogen and proton adsorption on a defective graphene surface served as additional example. The results of the QM/MM MD simulations provide detailed insight into the applicability of the employed link‐bond strategy when studying intercalation and adsorption properties of graphitic materials.