We use r2SCAN-rVV10/PAW600 as the main DFT-D method, where PAW600 means PAW pseudopotentials with 600 eV plane wave energy cutoff. It is universally the most accurate and reliable among available scalable methods. Robust method benchmarking is currently hardly possible due to lack of high quality experimental data and absence of computationally feasible higher-level theoretical approaches. All plane-wave calculations are performed in VASP 6 package. Because hybrid perovskites are very soft, their geometries cannot be efficiently optimized by to 1 meV/Ao by both IBRION=1,2. Consequently, we set the threshold to 3 meV/Ao for selected systems such as PEA and MBA and 5 meV/Ao for the rest. In these settings, the difference between R/S-MBA geometrical parameters is few percent. For isolated layers the periodic box in the nonperiodic dimension is 30 Ao. For MD of systems containing only heavy atoms such as Cs, Sn, I, the time step can be increased to 10 fs.
For calculations of clusters we use PBE/Def2-SVP for scalable calculations and PBE0/Def2-TZVP for accurate calculations as implemented in Gaussian 16 package.
See also technical details common for all CMSOS projects here.