R2scan-Based Composite Methods for Solid-State Calculations

Abstract In this work, we have extended the existing “sol-3c” composite methods to meta-GGA XC functionals using the r2SCAN one. The corresponding r2SCAN-based composite methods in their pure and hybrid HF/DFT variants have been developed in combination with double-ζ (sol-def2-mSVP) and triple-ζ (pob-TZVP-rev2) quality basis sets specifically adapted to solids. The r2SCAN “sol-3c/pob-3c” methods are validated and tested on benchmark sets containing both intermolecular adducts (S66 × 7), molecular crystals (X23, DMC8) and simple inorganic solids (SS20). They are then applied to selected applications of relevance for solid-state calculations such as the study of the energetic and structural properties of layered materials, the mechanical, electronic and vibrational properties of α-quartz, relative stability of all-silica zeolite polymorphs, α-quartz vs stishovite phase transition and the adsorption of small molecules on the surface of inorganic solids and in the pore of metal–organic frameworks. The new methods show broad applicability with accurate results and an adjustable and affordable computational cost.