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Are high-Z' polymorphs metastable? Insight from pharmaceutical polymorphs.

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The study investigated if crystal structures with more molecules (high-Z') are less stable. Analyzing 49 drug polymorphs revealed no direct link between Z' and crystal stability.

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Area of Science:

  • Crystallography
  • Solid-state chemistry
  • Computational chemistry

Background:

  • High-Z' polymorphs are theorized to be less stable than low-Z' forms.
  • This symmetry-stability relationship lacks experimental or computational validation.
  • Analyzing high-Z' structures is computationally challenging due to large atom counts.

Purpose of the Study:

  • To computationally assess the relationship between Z' and stability in drug polymorphs.
  • To determine if crystal structures with more molecules per asymmetric unit are inherently less stable.
  • To provide evidence for or against the fundamental hypothesis of symmetry-driven stability in molecular crystals.

Main Methods:

  • Utilized the CE-B3LYP method for efficient Lattice Cohesive Energy (LCE) estimation.
  • Analyzed 49 polymorphs across 15 different drugs.
  • Evaluated LCEs, Kitaigorodskii packing indices (KPI), molecular volumes, and crystal densities.

Main Results:

  • No direct correlation was found between Z' (number of molecules in the asymmetric unit) and polymorph stability.
  • Lattice cohesive energies did not consistently decrease with increasing Z'.
  • Kitaigorodskii packing indices, molecular volumes, and crystal densities also showed no clear trend with Z'.

Conclusions:

  • The hypothesis that high-Z' polymorphs are inherently less stable is not supported by this study.
  • Crystal stability in drug polymorphs is not directly dictated by the number of molecules in the asymmetric unit.
  • Further research may be needed to identify other factors governing polymorph stability.