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Our model shows quantitative agreement with experimental observations of the maximum phase-pure stoichiometric index (Ncrit) and explains the nonmonotonic evolution of the lattice parameters with increasing stoichiometric index (N). This model is generalizable to the entire family of q-2DPKs and can guide the design of photovoltaic and optical materials that combine the structural stability of the q-2DPKs while retaining the charge carrier properties of their 3D counterparts.Molecular rotors have attracted considerable interest for thei