Journal of the American Chemical Society · 2007 · 91 citations · 33 references
Natural SciencesChemistryMaterials ScienceChemical KineticsComputational ChemistryTheoretical ChemistryKinetic ModelingNucleationPolymorphic TransformationsReaction Coordinate AnalysisReaction MechanismsCrystallization KineticsLikelihood MaximizationNucleation PathwaysSolid-state TransformationSupramolecular Synthons
A molecular mechanism for nucleation for the solid-state polymorph transformation of terephthalic acid is presented. New methods recently developed in our group, aimless shooting and likelihood maximization, are employed to construct a model for the reaction coordinate for the two system sizes studied. The reaction coordinate approximation is validated using the committor probability analysis. The transformation proceeds via a localized, elongated nucleus along the crystal edge formed by fluctuations in the supramolecular synthons, suggesting a nucleation and growth mechanism in the macroscopic system.
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