The invention relates to methods of assessing the polymorphic form of a substance by assessing Raman-shifted radiation scattered by a particle of the substance. The method is useful, for example, for assessing particle sizes and size distributions in mixtures containing both particles of the substance and other materials. The invention also relates to methods of selecting and controlling polymorph formation by illuminating a material with non-resonant (i.e., non-absorbed) laser radiation as it is thermally driven through a phase transition temperature.
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